Accelerated discovery of a large family of quaternary chalcogenides with very low lattice thermal conductivity
Accelerated discovery of a large family of quaternary chalcogenides with very low lattice thermal conductivity
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DOI：
10.1038/s41524-021-00549-x
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发表时间：
2021-06-03
影响因子：
9.7
通讯作者：
Wolverton, Chris
中科院分区：
文献类型：
--
作者：
Pal, Koushik;Xia, Yi;Wolverton, Chris
高效热能管理装置（例如热电材料和隔离涂层）的开发通常依赖于具有低晶格导热系数（kappa (l)）的化合物。在这里，我们展示了使用高通量密度泛函理论 (DFT) 计算发现的 628 种热力学稳定的四元硫族化物大家族，AMM ' Q(3)（A=碱金属/碱土/后过渡金属；M/M '=过渡金属、镧系元素；Q=硫属元素）。我们通过使用 Peierls-Boltzmann 输运方程计算几种预测的稳定化合物的 kappa (l) 来验证这些材料中是否存在低 kappa (l)。我们的分析表明，低卡伯 (l) 源于增强声子散射的强晶格非谐性或导致晶体结构中多个散射通道的响尾阳离子的存在。我们的热电计算表明，一些预测的半导体可能具有高能量转换效率，其品质因数在接近 600 K 时超过 1。我们的预测表明，这些稳定的低 kappa (l) 化合物的合成和表征方面存在实验研究机会。
The development of efficient thermal energy management devices such as thermoelectrics and barrier coatings often relies on compounds having low lattice thermal conductivity (kappa (l)). Here, we present the computational discovery of a large family of 628 thermodynamically stable quaternary chalcogenides, AMM ' Q(3) (A=alkali/alkaline earth/post-transition metals; M/M ' =transition metals, lanthanides; Q=chalcogens) using high-throughput density functional theory (DFT) calculations. We validate the presence of low kappa (l) in these materials by calculating kappa (l) of several predicted stable compounds using the Peierls-Boltzmann transport equation. Our analysis reveals that the low kappa (l) originates from the presence of either a strong lattice anharmonicity that enhances the phonon-scatterings or rattler cations that lead to multiple scattering channels in their crystal structures. Our thermoelectric calculations indicate that some of the predicted semiconductors may possess high energy conversion efficiency with their figure-of-merits exceeding 1 near 600 K. Our predictions suggest experimental research opportunities in the synthesis and characterization of these stable, low kappa (l) compounds.