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Phonon anharmonicity of monoclinic zirconia and yttrium-stabilized zirconia

机译:单斜晶氧化锆和钇稳定氧化锆的声子非谐性

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摘要

Inelastic neutron scattering measurements on monoclinic zirconia (ZrO_2) and 8 mol% yttrium-stabilized zirconia were performed at temperatures from 300 to 1373wK. Temperature-dependent phonon densities of states (DOS) are reported, as are Raman spectra obtained at elevated temperatures. First-principles lattice dynamics calculations with density functional theory gave total and partial phonon DOS curves and mode Grüneisen parameters. These mode Grüneisen parameters were used to predict the experimental temperature dependence of the phonon DOS with partial success. However, substantial anharmonicity was found at elevated temperatures, especially for phonon modes dominated by the motions of oxygen atoms. Yttrium-stabilized zirconia (YSZ) was somewhat more anharmonic and had a broader phonon spectrum at low temperatures, owing in part to defects in its structure. YSZ also has a larger vibrational entropy than monoclinic zirconia.
机译:在300至1373wK的温度下对单斜晶氧化锆(ZrO_2)和8摩尔%的钇稳定的氧化锆进行非弹性中子散射测量。报告了与温度有关的声子密度(DOS),以及在高温下获得的拉曼光谱。用密度泛函理论进行的第一性原理晶格动力学计算给出了全部和部分声子DOS曲线以及模式Grüneisen参数。这些模式的Grüneisen参数用于部分成功预测声子DOS的实验温度依赖性。但是,在升高的温度下发现了很大的非谐性,特别是对于以氧原子的运动为主的声子模式。钇稳定的氧化锆(YSZ)在某种程度上更具非谐性,并且在低温下具有较宽的声子谱,这部分是由于其结构缺陷。 YSZ也比单斜晶氧化锆具有更大的振动熵。

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