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Convergence of multi-valley bands as the electronic origin of high thermoelectric performance in CoSb_3 skutterudites

机译:CoSb_3 skutterudites中多谷带的收敛作为高热电性能的电子起源

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摘要

Filled skutterudites R_xCo_4Sb_(12) are excellent n-type thermoelectric materials owing to their high electronic mobility and high effective mass, combined with low thermal conductivity associated with the addition of filler atoms into the void site. The favourable electronic band structure in n-type CoSb_3 is typically attributed to threefold degeneracy at the conduction band minimum accompanied by linear band behaviour at higher carrier concentrations, which is thought to be related to the increase in effective mass as the doping level increases. Using combined experimental and computational studies, we show instead that a secondary conduction band with 12 conducting carrier pockets (which converges with the primary band at high temperatures) is responsible for the extraordinary thermoelectric performance of n-type CoSb_3 skutterudites. A theoretical explanation is also provided as to why the linear (or Kane-type) band feature is not beneficial for thermoelectrics.
机译:填充的方钴矿R_xCo_4Sb_(12)由于其高的电子迁移率和高的有效质量,以及与将填料原子添加到空隙部位有关的低导热性,是极好的n型热电材料。 n型CoSb_3中有利的电子能带结构通常归因于导带最小处的三倍简并伴随着较高载流子浓度下的线性能带行为,这被认为与有效质量随掺杂水平的提高而增加有关。使用组合的实验和计算研究,我们相反地显示,具有12个导电载流子腔的次级导带(在高温下会与初级导带会聚)是n型CoSb_3方钴矿超常热电性能的原因。还提供了有关线性(或Kane型)能带特征为何对热电器件不利的理论解释。

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  • 来源
    《Nature Materials》 |2015年第12期|1223-1228|共6页
  • 作者单位

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,Materials Science, California Institute of Technology, Pasadena, California 91125, USA;

    Division of Chemistry and Chemical Engineering, California Institute of Technology, Pasadena, California 91125, USA;

    Department of Physics, University of North Texas, Denton, Texas 76203, USA,Department of Mechanical Engineering and Materials Science, Physics and Chemistry, Duke University, Durham, North Carolina 27708, USA;

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,Materials Science, California Institute of Technology, Pasadena, California 91125, USA,State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, Hubei 430070, China;

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,Materials Science, California Institute of Technology, Pasadena, California 91125, USA,Materials Research Center, Samsung Advanced Institute of Technology, Samsung Electronics, Suwon 443-803, South Korea;

    Department of Physics, University of North Texas, Denton, Texas 76203, USA;

    Department of Mechanical Engineering and Materials Science, Physics and Chemistry, Duke University, Durham, North Carolina 27708, USA;

    Department of Materials Science and Engineering, Northwestern University, Evanston, Illinois 60208, USA,Materials Science, California Institute of Technology, Pasadena, California 91125, USA;

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