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High-performance non-Fermi-liquid metallic thermoelectric materials
发布时间:2023-11-08

High-performance non-Fermi-liquid metallic thermoelectric materials

   Zirui Dong, Yubo Zhang, Jun Luo, Ying Jiang, Zhiyang Yu, Nan Zhao, Liusuo Wu, Yurong Ruan, Fang Zhang, Kai Guo, Jiye Zhang & Wenqing Zhang    
 

    npj Computational Materials 9: 41 (2023)
   doi.org/10.1038/s41524-023-01001-y
    Published online: 25 March 2023
   AbstractFull Text | PDF OPEN
  

  
Abstract: Searching for high-performance thermoelectric (TE) materials in the paradigm of narrow-bandgap semiconductors is hampered by a bottleneck. Here we report on the discovery of metallic compounds, TiFexCu2x?1Sb and TiFe1.33Sb, showing the thermopower exceeding many TE semiconductors and the dimensionless figure of merits zTs comparable with the state-of-the-art TE materials. A quasi-linear temperature (T) dependent electrical resistivity in 2–700?K and the logarithmic T-dependent electronic specific heat at low temperature coexist with the high thermopower, highlighting the strong intercoupling of the non-Fermi-liquid (NFL) quantum critical behavior of electrons with TE transports. Electronic structure analysis reveals a competition between the antiferromagnetic (AFM) ordering and Kondo-like spin compensation as well as a parallel two-channel Kondo effect. The T-dependent magnetic susceptibility agrees with the quantum critical scenario of strong local correlation. Our work demonstrates the correlation among high TE performance, NFL quantum criticality, and magnetic fluctuation, which opens up directions for future research.
摘要:  在窄带隙半导体范式中寻找高性能热电(TE)材料触及了瓶颈。在本文中,我们报道了两种金属化合物, TiFexCu2x?1Sb和TiFe1.33Sb,其热电势超过了很多TE半导体,并且无量纲热电性能指标zTs与最先进的热电材料相当。在2-700 K范围内存在准线性温度(T)依赖的电阻率,以及在低温下对数T相关的电子比热,与高温电势共存,这突显了电子的非费米液体(NFL)量子临界行为与TE输运的强耦合。电子结构分析揭示了反铁磁(AFM)序和近藤类自旋补偿之间的竞争,以及平行的双通道近藤效应。T相关的磁化率与强局部关联的量子临界情形一致。我们的工作证明了高TE性能、NFL量子临界性和磁涨落之间的关联,为未来的研究开辟了方向。
Editorial Summary

New frontiers of thermoelectric materials: Non-fermi liquid metals 

TE materials have been studied and developed for 200 years since the Seebeck effect was discovered in 1821. Due to the promising applications of TE materials in waste heat power generation and solid-state refrigeration, persistent efforts have been made to improve TE performance. The best TE materials at present, such as Bi2Te3, PbTe, GeTe, and CoSb, are all heavily-doped narrow-bandgap semiconductors. In addition, reliably reproducible zT is around 2.0, the reported zT values above 2.0 are often in debate, and all belong to heavily-doped narrow-bandgap semiconductors. Therefore, it seems desperately needed to break through the limitation of narrow-bandgap semiconductors for discovering high-performance TE materials. In this work, a team led by Prof. Jun Luo from Shanghai University and Prof. Wenqing Zhang from Southern University of Science and Technology, demonstrated that a few Heusler-like materials, TiFexCu2x?1Sb (x?=?0.70, 0,75, 0.80) and TiFe1.33Sb, show peculiar NFL metallic transport together with promising TE performance. The study revealed that the NFL metal showing a quantum critical behavior may be a type of high-performance TE material. The random filling of Fe/Cu atoms on the equivalent 4c/4d sites of the Heusler metals TiFexCu2x?1Sb and TiFe1.33Sb, leads to the structure disorder, strong magnetic fluctuation, and quantum critical behavior of these non-conventional metals. The Seebeck coefficient of TiFexCu2x?1Sb and TiFe1.33Sb increases continuously with the increase of temperature, while a low resistivity is maintained at the same time. Combined with the very low thermal conductivity due to the disordered structure, the TiFexCu2x?1Sb and TiFe1.33Sb samples achieve the TE performance comparable to or even better than the traditional TE semiconductors. Among them, the TiFe0.7Cu0.4Sb sample shows a Seebeck coefficient of 194 V/K at 700?K and a zT value of 0.75 at 973?K, suggesting the potential to search for high-performance TE materials along this direction. This work demonstrates the correlation among high TE performance, NFL quantum criticality, and magnetic fluctuation, which opens up directions for future research.
热电材料新蓝海:非费米液体金属

自1821年发现Seebeck效应以来,热电材料已经被研究了200多年。由于热电材料在废热发电和固态制冷等领域有着广泛的应用前景,人们一直在努力提高热电材料的性能。目前最好的热电材料,如Bi2Te3、PbTe、GeTe和CoSb等,都是重掺杂的窄带隙半导体。此外,文献报道的可靠可重复性的zT值约为2.0,超过2.0的zT值经常存在争议,并且都属于重掺杂窄带隙半导体。因此,研究上似乎迫切需要打破窄带隙半导体的限制,以发现新型的高性能热电材料。在本工作中,来自上海大学骆军教授、南方科技大学张文清教授团队,发现了一些类似Heusler的材料,TiFexCu2x?1Sb(x=0.70,0,75,0.80)和TiFe1.33Sb,它们表现出特殊的非费米液体(NFL)金属输运和良好的热电性能。研究发现,具有量子临界行为的NFL金属可能是一种高性能热电材料。在Heusler金属TiFexCu2x?1Sb和TiFe1.33Sb的等效4c/4d位点上,Fe/Cu原子的随机填充,导致了这些非常规金属的结构无序、强磁涨落和量子临界行为。TiFexCu2x?1Sb和TiFe1.33Sb的Seebeck系数随着温度的升高而不断增加,同时保持了较低的电阻率。结合由于无序结构导致的非常低的热导率,TiFexCu2x?1Sb和TiFe1.33Sb样品实现了与传统热电半导体相当甚至更好的热电性能。其中,TiFe0.7Cu0.4Sb样品在700 K时的Seebeck系数为194 V/K,在973 K时的zT值为0.75,这表明了沿这个方向寻找高性能TE材料的潜力。该研究证明了高热电性能、NFL量子临界性和磁涨落之间的相关性,这为未来的研究开辟了方向。

 
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