高压下CeO2晶格动力学及热输运性质第一性原理研究

First Principles Study on Lattice Dynamics and Thermal Transport Properties of CeO2 under High Pressure

  • 摘要: 基于密度泛函理论和玻尔兹曼输运方程,研究CeO2高压下的弹性性质、热力学性质以及晶格热导率。CeO2在0~30 GPa以内保持晶格动力学稳定性。300 K时,CeO2的晶格热导率在压力为0、10、20和30 GPa时分别为10.02、14.92、20.97和26.75 W·(m∙K)–1,声学声子对CeO2晶格热导率的贡献大于光学声子。在高压下,声子弛豫时间显著增加是CeO2热导率增加的主要原因。作为对比,采用基于机器学习的从头算分子动力学方法(AIMD)计算了CeO2在零压下的声子散射和晶格热导率,在300 K和0 GPa条件下AIMD得到的晶格热导率为11.19 W·(m∙K)–1

     

    Abstract: Based on density functional theory and Boltzmann transport equation, this paper investigates the elastic properties, thermodynamic properties, and lattice thermal conductivity of CeO2 under high pressure. CeO2 exhibits lattice dynamic stability within 0 GPa-30 GPa. At 300 K, the lattice thermal conductivity of CeO2 is 10.02, 14.92, 20.97, and 26.75 W·(m∙K)–1 at 0, 10, 20, and 30 GPa, respectively. Acoustic phonons contribute more to the lattice thermal conductivity of CeO2 than optical phonons. The increase in lifetimes under high pressure is the main reason for the significant increase in thermal conductivity of CeO2. As a comparison, the Ab-initio Molecular Dynamics (AIMD) based on machine learning is used to simulate the phonon and lattice thermal conductivity of CeO2 at 0 GPa. The lattice thermal conductivity obtained by AIMD at 300 K and 0 GPa is 11.19 W·(m∙K)–1.

     

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