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中国物理学会期刊

BaVS3晶格动力学研究

CSTR: 32037.14.aps.57.3709

The lattice dynamics of BaVS3 compound

CSTR: 32037.14.aps.57.3709
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  • 采用基于密度泛函理论的平面波赝势方法,在局域密度近似下采用线性响应的密度泛函微扰理论研究了具有六角结构的BaVS3化合物的晶格动力学性质,得到了整个声子谱.计算得到的Γ点拉曼频率和实验数据进行了比较,其中E22g模、A1g模和实验测量值符合得比较好.对于E32g模,采用线性响应计算的结果与实验值差别较大.对该模应用冻结声子方法研究后认为差异主要是由于E32g模的较强的非谐性引起的.此外V原子在平面内的振动模E12u出现了虚频.虚频的出现预示着六角相的BaVS3结构的不稳定性,从而很好地解释了该材料由六角相到正交相的结构相变.

     

    The lattice dynamics of hexagonal perovskite BaVS3 compound is studied by first-principles calculations based on the ab initio pseudopotential and plane wave basis. Phonon spectra throughout the Brillouin zone are obtained using the density-functional perturbation method within the framework of linear response theory. The calculated frequencies of the Raman active modes are compared with the experimental measurements. For E22g and A1g modes, our calculated values are in good agreement with the experiment. But for E32g mode, the value of the calculated frequency differs significantly from the experiment. After further calculation using the frozen-in phonon method, we suggest that this difference is caused by the large anharmonicity of E32g mode. The most prominent feature of the phonon spectrum is that there appears the imaginary frequency for E12u mode, which involves the planar vibration of the vanadium atoms. The appearance of imaginary frequency for E12u mode indicates the planar instability of hexagonal BaVS3 crystal structure. We believe that this soft mode is responsible for the observed hexagonal-orthorhombic phase transition.

     

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