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InTe 晶体电热输运性能的研究

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LIN Peijian
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070205 凝聚态物理
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07 理学
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       热电材料是一种能够实现电能与热能直接相互转化的材料,其在新能源领域中扮演着重要角色。InTe近年来因其具有极低的晶格热导率而受到广泛的关注,但其研究主要集中在对多晶样品的掺杂调控和热电性能优化方面,而针对InTe 强各向异性的本征电热输运性能和机理研究却十分稀少 。因此,我们对InTe单晶生长工艺和单晶电热输运特性展开系统的研究,为利用各向异性提升其热电性能提供理论依据。

       通过布里奇曼法成功生长大尺寸高质量的 InTe 单晶,首次基于单晶进行了全温度段的热电各向异性的完整表征。发现其[110]方向在全温度段均保持着高电导率、低热导率的各向异性。通过第一性原理计算,我们发现其电学各向异性是由价带顶不对称的能带结构导致的有效质量各向异性所引起的;声子色散谱的计算表明其群速度以及格林奈森常数存在各向异性,[110] 方向的低群速度以及高格林奈森常数导致 [110] 方向具有比[001] 方向更低的热导率。

       通过单晶不同部位性能测试发现,单晶生长方向存在In1+空位梯度并导致单晶不同位置载流子浓度存在差别,进而引起单晶顶部和底部的热电性能存在明显的差异。利用In 蒸汽退火处理,可以有效改善In1+空位分布不均的现象,实现晶体载流子浓度的可控调节,使单晶底部与顶部热电性能趋于一致。经过In蒸汽退火后,InTe[110]方向最高zT值从773 K转移到600 K,平均zT值得以提升40%并最终达到0.7,是目前InTe体系中最高的平均zT值。    

        低温下InTe 晶体电输运存在对载流子浓度的依赖关系,较高载流子浓度时(~6.6×1019 cm-3)呈现金属导电特性,较低载流子浓度(~1.1×1019 cm-3)时则会呈现出类电荷密度波转变的导电特性。变温PXRD、ARPES 以及 Raman光谱的分析显示,在不同温度下,两种具有不同导电行为的样品的结构、能带以及声子振动模式并无明显区别,表明其电阻异常行为与电荷密度波关联性不大,具体原因还需进一步分析。

Other Abstract

Thermoelectric(TE) material is a kind of material that can realize the direct mutual conversion between electricity and thermal energy, which plays an essential role in energy. InTe has received extensive attention in recent years due to its extremely low lattice thermal conductivity. Moreover, the research interest was mainly focused on the TE performance optimization of polycrystalline samples by doping. However, the study on its intrinsic anisotropic electrical and thermal transport properties and the mechanism is rare. Therefore, we systematically investigated the growth process and the electrical and thermal transport characteristics of InTe single crystal, which can provide a theoretical basis for using transport anisotropy to improve its TE performance.

Large-scale and high-quality InTe single crystals were successfully grown by the Bridgman method. The TE anisotropy of the whole temperature range was fully characterized for the first time based on single crystals. Its [110] direction maintains high electrical conductivity and low thermal conductivity in the whole temperature range. Based on the first-principles calculation, we found that the reason for its electrical anisotropy is the asymmetric energy band structure at the valence band maximum, resulting in different effective masses in two directions. The calculation of the phonon dispersion spectrum shows that the group velocity and the Gruneisen parameter are also anisotropic. The low group velocity and high Gruneisen parameter in the [110] direction result in lower thermal conductivity than in the [001] direction.

Through the performance test of different parts of the single crystal, it is found that there is a gradient of In1+  vacancy concentration in the growth direction of the single crystal, which leads to differences in the carrier concentration at different positions of the single crystal.
 Therefore, there is a noticeable TE properties difference between the top and bottom sides of the crystal. The use of In steam annealing treatment can effectively improve the heterogeneous distribution of In1+ vacancies, and realize the controllable adjustment of the carrier concentration, therefore making TE performance of the bottom and top side samples tend to be consistent. After In steam annealing, the highest zT in the [110] direction shifted from 773 K to 600 K, and the average zT increased by 40% and finally reached 0.7, the highest average zT in the current InTe system.

The electrical transport of InTe crystal at low temperature is dependent on the carrier concentration. The crystal with a higher carrier concentration(6.6×1019 cm-3) exhibits metal-like conductivity, and the crystal with a lower carrier concentration(1.1×1019 cm-3)  manifests a charge density wave (CDW)-like conductive behavior. Using temperature-variable PXRD, ARPES, and Raman spectroscopy analysis, we found no apparent difference in the structures, energy bands, and phonon vibration modes between two different conductive behaviors samples at varying temperatures. These results indicate that their anomalous resistance behaviors were independent of charge density waves(CDW).

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林培坚. InTe 晶体电热输运性能的研究[D]. 深圳. 南方科技大学,2022.
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