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中国物理学会期刊

具有超低晶格热导率与优异热电性能的准一维材料Bi4RuI2的第一性原理研究

First-principles study on the ultra-low lattice thermal conductivity and excellent thermoelectric properties of the quasi-one-dimensional Bi4RuI2

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  • 准一维材料因其维度降低和链间较弱的范德华相互作用,为实现超低晶格热导率的热电应用提供了优异平台. 本文利用第一性原理计算结合玻尔兹曼输运理论,探究了准一维材料Bi4RuI2的热电输运性质. 计算结果表明,Bi4RuI2表现出极低的本征链间和链内晶格热导率,温度为300(800) K时分别为0.349和1.851(0.131和0.714) W/mK. Bi4RuI2极低的热导率源于较小的声子群速度与较强的晶格非谐性,这可以归因于较重的组成元素、复杂的晶体结构、声子的避免交叉、孤对电子以及多种键合相互作用. 由于一维共价链间的范德华相互作用较弱,Bi4RuI2的晶格热导率表现出明显的各向异性,链间方向的热导率明显低于链内方向. 此外,较高的功率因子和较低的晶格热导率,使得Bi4RuI2具有高的热电优值,表现出良好的热电性能. 在n型载流子掺杂下,温度为800 K时链间和链内方向最大热电优值ZT分别可以达1.59和2.54. 这些理论发现表明准一维Bi4RuI2是一种潜在的高性能热电低维材料,在亚纳米器件中有良好的应用前景.

    The quasi-one-dimensional (quasi-1D) materials serve as an excellent platform to realize ultra-low lattice thermal conductivity for thermoelectric applications, attributed to their reduced dimensionality and weak interchain van der Waals (vdW) interactions. Herein, utilizing first-principles calculations and Boltzmann transport theory, we explore the thermoelectric transport properties of the quasi-1D Bi4RuI2. Our calculation results indicate that Bi4RuI2 exhibits extraordinarily low intrinsic interchain and intrachain lattice thermal conductivity of 0.349 and 1.851 (0.131 and 0.714) W/mK at 300 (800) K, respectively. The damped thermal transport properties originate from the low phonon group velocity and large lattice anharmonicity due to the heavy component elements, complex crystal structure, avoided-crossing effects, lone-pair electrons, and bonding hierarchy. Notably, the lattice thermal conductivity exhibits pronounced anisotropy, which is obviously smaller along the interchain direction than that along the intrachain direction due to the weaker vdW interactions between the 1D covalent chains. Furthermore, Bi4RuI2 achieves high figure-of-merit (ZT) values due to the high power-factor and low lattice thermal conductivity, which reaches maximum values of about 1.59 and 2.54 at 800 K along the interchain and intrachain directions by n-type carrier doping. These findings establish quasi-1D Bi4RuI2 as a promising candidate for high-performance low-dimensional thermoelectric materials.

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