Effect of pressure on electronic and thermoelectric properties of magnesium silicide: A density functional theory study

We study the effect of pressure on electronic and thermoelectric properties of Mg_2Si using the density functional theory and Boltzmann transport equations. The variation of lattice constant, band gap, bulk modulus with pressure is also analyzed. Further, the thermoelectric properties(Seebeck coefficient, electrical conductivity, electronic thermal conductivity) have been studied as a function of temperature and pressure up to 1200 K. The results show that Mg_2Si is an n-type semiconductor with a band gap of 0.21 eV. The negative value of the Seebeck coefficient at all pressures indicates that the conduction is due to electrons. With the increase in pressure, the Seebeck coefficient decreases and electrical conductivity increases. It is also seen that, there is practically no effect of pressure on the electronic contribution of thermal conductivity.The paper describes the calculation of the lattice thermal conductivity and figure of merit of Mg_2Si at zero pressure. The maximum value of figure of merit is attained 1.83 × 10~(-3) at 1000 K. The obtained results are in good agreement with the available experimental and theoretical results.     

N-type core-shell heterostructured Bi2S3@Bi nanorods/polyaniline hybrids for stretchable thermoelectric generator

With the growing need on distributed power supply for portable electronics,energy harvesting from environment becomes a promising solution.Organic thermoelectric(TE)materials have advantages in intrinsic flexibility and low thermal conductivity,thus hold great prospect in applications as a flexible power generator from dissipated heat.Nevertheless,the weak electrical transport behaviors of organic TE materials have severely impeded their development.Moreover,compared with p-type organic TE materials,stable and high-performance n-type counterparts are more difficult to obtain.Here,we developed a n-type polyaniline-based hybrid with core-shell heterostructured Bi;S;@Bi nanorods as fillers,showing a Seebeck coefficient-159.4μV/K at room temperature.Further,a couple of n/p legs from the PANI-based hybrids were integrated into an elastomer substrate forming a stretchable thermoelectric generator(TEG),whose function to output stable voltages responding to temperature differences has been demonstrated.The in situ output performance of the TEG under stretching could withstand up to 75%elongation,and stability test showed little degradation over a one-month period in the air.This study provides a promising strategy to develop stable and high thermopower organic TEGs harvesting heat from environment as long-term power supply.     

Thermoelectric performance of XI2 (X = Ge,Sn, Pb) bilayers

We study the thermal and electronic transport properties as well as the thermoelectric (TE) performance of three two-dimensional (2D) XI₂ (X=Ge, Sn, Pb) bilayers using density functional theory and Boltzmann transport theory. We compared the lattice thermal conductivity, electrical conductivity, Seebeck coefficient, and dimensionless figure of merit (ZT) for the XI₂ monolayers and bilayers. Our results show that the lattice thermal conductivity at room temperature for the bilayers is as low as ~1.1 W·m^{-1·K-1-1.7 W}·m^{-1·K-1, which is about 1.6 times as large as the monolayers for all the three materials. Electronic structure calculations show that all the} XI₂ bilayers are indirect-gap semiconductors with the band gap values between 1.84 eV and 1.96 eV at PBE level, which is similar as the corresponding monolayers. The calculated results of ZT show that the bilayer structures display much less direction-dependent TE efficiency and have much larger n-type ZT values compared with the monolayers. The dramatic difference between the monolayer and bilayer indicates that the inter-layer interaction plays an important role in the TE performance of XI₂, which provides the tunability on their TE characteristics.     

First principle investigation of the electronic and thermoelectric properties of Mg_2C

In this paper, electronic and thermoelectric properties of Mg_2C are investigated by using first principle pseudo potential method based on density functional theory and Boltzmann transport equations. We calculate the lattice parameters,bulk modulus, band gap and thermoelectric properties(Seebeck coefficient, electrical conductivity, and thermal conductivity) of this material at different temperatures and compare them with available experimental and other theoretical data. The calculations show that Mg_2C is indirect band semiconductor with a band gap of 0.75 eV. The negative value of Seebeck coefficient shows that the conduction is due to electrons. The electrical conductivity decreases with temperature and Power factor(PF) increases with temperature. The thermoelectric properties of Mg_2C have been calculated in a temperature range of 100 K–1200 K.     

Electric and thermal transport properties of topological insulator candidate LiMgBi

We report the transport properties of a topological insulator candidate, LiMgBi. The electric resistivity of the title compound exhibits a metal-to-semiconductor-like transition at around 160 K and tends to saturation below 50 K. At low temperatures, the magnetoresistance is up to ~260% at 9 T and a clear weak antilocalization effect is observed in the low magnetic-field region. The Hall measurement reveals that LiMgBi is a multiband system, where hole-type carriers (n_h~10¹⁸ cm^-3) play a major role in the transport process. Remarkably, LiMgBi possess a large Seebeck coefficient (~440 μV/K) and a moderate thermal conductivity at room temperature, which indicate that LiMgBi is a promising candidate in thermoelectric applications.     

Strong Anisotropic Thermal Conductivity in Polycrystalline Layers of (AgxSn1-xS)1.2(TiS2)2 with Prospects Toward Improved Thermoelectric Performance

Anisotropic tuning is of crucial importance for designing and developing high-performance thermoelectric materials. Here, a prominent anisotropic thermoelectric characteristic of Ag-substituted misfit-layered (SnS)_1.2(TiS₂)₂ alloys is investigated in the perpendicular (in-plane) and parallel (out-of-plane) to the pressing direction. In the in-plane direction, the (Ag_xSn_1-xS)_1.2(TiS₂)₂ alloys possess a highest power factor of 0.86 mW K⁻² m⁻¹ at 520 K, while in the out-of-plane direction the lowest lattice thermal conductivity (0.37 W K⁻¹ m⁻¹) is achieved, which is driven by the natural intercalated structure where the out-of-plane phonon is strongly scattered without affecting the in-plane mobility. Moreover, along the in-plane orientation, the introduced point defects due to the substitution of Sn by Ag trigger a significant reduction of lattice thermal conductivity. In contrast, along the out-of-plane orientation, the decreased carrier concentration enables a large Seebeck coefficient and power factor, ultimately ensuring high thermoelectric performance. The present finding in the misfit-layered chalcogenide opens up a new route to manipulating thermoelectrics via anisotropy engineering.     

具有本征低晶格热导率的硫化银快离子导体的热电性能

硫化银(Ag_2S)是一种典型的快离子导体材料,前期关于Ag_2S的研究主要集中在光电和生物等领域.最近的研究表明, a-Ag_2S具有和金属一样的良好延展性和变形能力.但是, Ag_2S的热电性能尚无公开报道.本工作合成了单相Ag_2S化合物,系统研究了其在300—600 K范围的物相变化、离子迁移特性和电热输运性质.研究发现, Ag_2S在300—600 K温度区间表现出半导体的电输运性质.由于单斜-体心立方相晶体结构转变, Ag_2S的离子电导率、载流子浓度、迁移率、电导率、泽贝克系数等性质在455 K前后出现急剧变化.在550 K, Ag_2S的功率因子最高可达5μW·cm~(–1)·K~(–2). Ag_2S在300—600 K温度区间均表现出本征的低晶格热导率(低于0.6 W·m~(–1)·K~(–1)). S亚晶格中随机分布的类液态Ag离子是导致b-Ag_2S体心立方相具有低晶格热导率的主要原因.在573 K, Ag_2S的热电优值可达0.55,与Ag_2Se, Ag_2Te, CuAgSe等已报道的Ag基快离子导体热电材料的性能相当.     

金属有机物化学气相沉积生长GaN薄膜的室温热电特性研究

采用金属有机物化学气相沉积技术生长了不同掺杂浓度的GaN薄膜, 并且通过霍尔效应测试和塞贝克效应测试, 表征了室温下GaN薄膜的载流子浓度、迁移率和塞贝克系数. 在实验测试的基础上, 计算了GaN薄膜的热电功率因子, 并且结合理论热导率确定了室温条件下GaN薄膜的热电优值(ZT). 研究结果表明: GaN薄膜的迁移率随着载流子浓度的增加而减小, 电导率随着载流子浓度的增加而增加; GaN 薄膜材料的塞贝克系数随载流子浓度的增加而降低, 其数量级在100–500 μV/K范围内; GaN薄膜材料在载流子浓度为1.60×10¹⁸ cm^-3时, 热电功率因子出现极大值4.72×10^-4 W/mK²; 由于Si杂质浓度的增加, 增强了GaN薄膜中的声子散射, 使得GaN薄膜的热导率随着载流子浓度的增加而降低. GaN薄膜的载流子浓度为1.60×10¹⁸ cm^-3时, 室温ZT达到极大值0.0025.     

高压烧结对n型PbTe基材料热电性能的影响

 采用高压烧结技术制备了按偏离化学计量比配制的PbTe基热电材料（Pb_0.55Te_0.45），重点研究了烧结压力对材料热电性能的影响。研究结果表明：高压烧结过程能有效降低材料中的晶格缺陷，从而显著改变样品中的载流子浓度及其迁移率。与未经烧结的常压熔融样品相比，高压烧结样品的Seebeck系数得到大幅提高，电导率略有降低，室温热导率降低了50%，所以高压烧结样品的品质因子得到较大提高。当烧结压力为2 GPa时，所得样品在700 K时其品质因子达到0.59，相比未经烧结的常压熔融样品提高了150%。     

Electrical and thermal transport properties of CdO ceramics

High temperature electrical and thermal transport properties, that is, electrical conductivity, Seebeck coefficient and thermal conductivity, of CdO ceramics have been investigated. Because of the good electrical properties and low thermal conductivity, the dimensionless figure-of-merit ZT of the CdO ceramics reaches 0.34 at 1023 K. This value is comparable to the best reported ZT for the n-type oxide ceramic thermoelectric materials and remains as potential to be further improved by porosity controlling or nanostructuring.     

β型锑烯热电输运性质的第一性原理研究

利用第一性原理与半经典玻尔兹曼方程，计算并分析β型锑烯的声子色散、声子群速度、声子弛豫时间、晶格热导率及不同温度下的塞贝克系数、电导率和电子热导率随化学势的变化；结果表明：β型锑烯由于非平面六角结构，三支声学声子在Γ点附近均呈线性变化；声学声子对整个晶格热导率的贡献高达96.68%，而光学声子仅仅占到3.32%；由于较大的声光带隙（a-o gap）导致LA支在声子群速度和弛豫时间中占据主导地位，从而增大了LA支声子对整个热导的贡献；热电优值随温度的升高而增大，在费米面附近其绝对值最大可达0.275.     

I型锗基笼合物Ba8Ga16-xSbxGe30的合成及热电性能

用高温熔融结合放电等离子烧结（SPS）方法合成了Sb掺杂的单相n型Ba8Ga16-xSbxGe30化合物，探索了Sb对Ga的取代对其热电性能的影响规律．研究结果表明：随着Sb取代分数x的增加，Seebeck系数逐渐降低，Seebeck系数峰值对应的温度向低温方向偏移．电导率随着x的增加先增大后减小，当x=2时达到最大值．Sb取代Ga后对化合物的热性能有较大影响，其热导率和晶格热导率都有不同程度的降低．在所有n型Ba8Ga16-xSbxGe30化合物中，Ba8Ga14Sb2Ge30化合物的ZT值最大，在950K左右其最大ZY值达1．1．     

N型稀磁半导体Ge_(0.96–x) Bi_xFe_(0.04)Te薄膜的磁电性质研究

GeTe基稀磁半导体材料因具有可独立调控载流子浓度和磁性离子浓度的特性而受到广泛关注.本文利用脉冲激光沉积技术制备了该体系的单晶外延薄膜,并通过高价态Bi元素部分取代Ge元素的方法实现了材料中载流子类型从空穴向电子的转变,即制备出N型GeTe基稀磁半导体.测量结果表明,无论是室温还是低温下的Hall电阻曲线皆呈现负斜率,说明体系中载流子是电子;并且当Bi掺杂量达到32%时,电子浓度为10~(21)/cm~3.变温输运性质的测量证明体系的输运行为呈现半导体特征.通过测量低温10 K下的绝热磁化曲线,在高Bi掺杂体系中观测到了明显的铁磁行为,而低于32%Bi掺杂量的体系中未观察到.这一结果说明,高掺杂Bi的替代导致载流子浓度的增加,促进了载流子传递Ruderman-Kittel-Kasuya-Yoshida相互作用,使得分散的Fe-Fe之间产生磁耦合作用,进而形成铁磁有序态.     

Ⅰ型锗基笼合物Ba8Ga16-xSbxGe30的合成及热电性能

用高温熔融结合放电等离子烧结(SPS)方法合成了Sb掺杂的单相n型Ba8Ga16-xSbxGe30化合物,探索了Sb对Ga的取代对其热电性能的影响规律.研究结果表明随着Sb取代分数x的增加,Seebeck系数逐渐降低,Seebeck系数峰值对应的温度向低温方向偏移.电导率随着x的增加先增大后减小,当x=2时达到最大值.Sb取代Ga后对化合物的热性能有较大影响,其热导率和晶格热导率都有不同程度的降低.在所有n型Ba8Ga16-xSbxGe30化合物中,Ba8Ga14Sb2Ge30化合物的ZT值最大,在950 K左右其最大ZT值达1.1.     

Ag-ZnO纳米复合热电材料的制备及其性能研究

ZnO是一类具有潜力的热电材料, 但其较大声子热导率影响了热电性能的进一步提高. 纳米复合是降低热导率的有效途径. 本文以醋酸盐为前驱体, 溶胶-凝胶法制备了Ag-ZnO纳米复合热电材料. 扫描电镜照片显示ZnO颗粒呈现多孔结构, Ag纳米颗粒分布于ZnO的晶粒之间. Ag-ZnO纳米复合材料的电导率比未复合ZnO材料高出100倍以上, 而热导率是未复合ZnO材料的1/2. 同时, 随着Ag添加量的增加, 赛贝克系数的绝对值逐渐减小. 综合以上原因, 添加7.5%mol Ag的Ag-ZnO纳米复合材料在700 K时的热电优值达到0.062, 是未复合ZnO材料的约25倍. 在ZnO基体中添加导电金属颗粒有利于产生导电逾渗通道, 提高材料体系的电导率, 但同时导致赛贝克系数的绝对值减小. 总热导率的差异来源于声子热导率的差异. 位于ZnO晶界的纳米Ag颗粒, 有利于降低声子热导率. 关键词： 热电材料 ZnO 纳米复合 热导率     

Ca2+掺杂对CdO多晶热电性能的影响

以CaCO₃作为Ca²⁺源, 利用传统固相烧结法制备了Cd_1-xCa_xO (x=0, 0.01, 0.03, 0.05) 多晶块体样品并研究了Ca²⁺掺杂对CdO高温热电性能的影响. CaCO₃的掺入会导致CdO多晶载流子浓度降低, 使Cd_1-xCa_xO的电阻率ρ和塞贝克系数的绝对值|S|增大、电子热导率κ_e减小. 同时, 在CdO中掺入CaCO₃会引入点缺陷和气孔并可抑制CdO晶粒长大、晶界增多, 从而增加了对声子的散射, 使样品的声子热导率κ_p减小. 由于总热导率的大幅降低, Cd_0.99Ca_0.01O多晶样品在1000 K时的热电优值ZT可达0.42, 比本征CdO提高了约27%, 为迄今n型氧化物热电材料报道的最好结果之一.     

Thermoelectric properties of Li-doped Sr_(0.7)Ba_(0.3)Nb_2O_(6-δ) ceramics

Thermoelectric properties of Li-dopedSr_(0.7)Ba_(0.3)Nb_2O_(6-δ)ceramics were investigated in the temperature range from 323 K to 1073 K. The electrical conductivity increases significantly after lithium interstitial doping. However, both of the magnitudes of Seebeck coefficient and electrical conductivity vary non-monotonically but synchronously with the doping contents, indicating that doped lithium ions may not be fully ionized and oxygen vacancy may also contribute to carriers. The lattice thermal conductivity increases firstly and then decreases as the doping content increases, which is affected by competing factors.Thermoelectric performance is enhanced by lithium interstitial doping due to the increase of the power factor and the thermoelectric figure of merit reaches maximum value(0.21 at 1073 K) in the sample Sr_(0.70)Ba_(0.30)Li_(0.10)Nb_2O_6.     

Advances in thermoelectric (GeTe)x(AgSbTe2)100-x

The (GeTe)_x(AgSbTe₂)_100-x alloys, also called TAGS-x in short, have long been demonstrated as a promising candidate for thermoelectric applications with successful services as the p-type leg in radioisotope thermoelectric generators for space missions. This largely stems from the complex band structure for a superior electronic performance and strong anharmonicity for a low lattice thermal conductivity. Utilization of the proven strategies including carrier concentration optimization, band and defects engineering, an extraordinary thermoelectric figure of merit, zT, has been achieved in TAGS-based alloys. Here, crystal structure, band structure, microstructure, synthesis techniques and thermoelectric transport properties of TAGS-based alloys, as well as successful strategies for manipulating the thermoelectric performance, are surveyed with opportunities for further advancements. These strategies involved are believed to be in principle applicable for advancing many other thermoelectrics.     

Synthesis and thermoelectric properties of Bi-doped SnSe thin films

Bi doped n-type SnSe thin films were prepared by chemical vapor deposition (CVD) and their structure and thermoelectric properties were studied. The x-ray diffraction patterns, x-ray photoelectron spectroscopy, and microscopic images show that the prepared SnSe thin films were composed of pure SnSe crystals. The Seebeck coefficients of the Bi-doped SnSe were greatly improved compared to that of undoped SnSe thin films. Specifically, Sn_0.99Bi_0.01Se thin film exhibited a Seebeck coefficient of -905.8μV·K^-1 at 600 K, much higher than 285.5 μV·K^-1 of undoped SnSe thin film. Further first-principles calculations reveal that the enhancement of the thermoelectric properties can be explained mainly by the Fermi level lifting and the carrier pockets increasing near the Fermi level due to Bi doping in the SnSe samples. Our results suggest the potentials of the Bi-doped SnSe thin films in thermoelectric applications.     

Cu对用于高速相变存储器的Sb2Te薄膜的结构及相变的影响研究

采用原位X射线衍射仪、拉曼光谱仪和X射线反射仪分别研究了Cu-Sb₂Te 薄膜的微结构、成键结构和结晶前后的密度变化. Sb₂Te薄膜的结晶温度随着Cu含量的增加而增大. 在10 at.%和14 at.% Cu的Sb₂Te薄膜中, Cu与 Te 成键, 结晶相由六方相的Cu₇Te₄、菱形相的Sb及六方相的Sb₂Te构成. 10 at.% 和14 at.% Cu 的Sb₂Te薄膜在结晶前后的厚度变化分别约为3.2%和 4.0%, 均小于传统的Ge₂Sb₂Te₅ (GST)薄膜. 制备了基于Cu-Sb₂Te薄膜的相变存储单元, 并测试了其器件性能. Cu-Sb₂Te器件均能在10 ns的电脉冲下实现可逆SET-RESET操作. SET和RESET操作电压随着Cu含量的增加而减小. 疲劳测试结果显示, Cu 含量为10 at.%和14 at.%的PCRAM单元的循环操作次数分别达到1.3×10⁴和1.5×10⁵, RESET和SET态的电阻比值约为100. Cu-Sb₂Te可以作为应用于高速相变存储器(PCRAM)的候选材料.