The effect of Te doping on the electronic structure and thermoelectric properties of SnSe

SnSe_1−xTe_x (x=0, 0.0625) bulk materials were fabricated by melting Sn, Se and Te powders and then hot pressing them at various temperatures. The phase compositions of the materials were determined by X-ray diffraction (XRD) and the crystal lattice parameters were refined by the Rietveld method performed with DBWS. XRD analysis revealed that the grains in the materials preferentially grew along the (l 0 0) directions. The structural behavior of SnSe_1−xTe_x (x=0, 0.0625) was calculated using CASTEP package provided by Materials Studio. We found that the band gap of SnSe reduced from 0.643 to 0.608 eV after Te doping. The calculated results were in good agreement with experimental results. The electrical conductivity and the Seebeck coefficient of the as-prepared materials were measured from room temperature to 673 K. The maximum power factor of SnSe is ∼0.7 μW cm⁻¹K⁻² at 673 K.     

High thermoelectric performance and low thermal conductivity in K-doped SnSe polycrystalline compounds

SnSe single crystal showed a high thermoelectric zT of 2.6 at 923 K mainly due to an extremely low thermal conductivity 0.23 W m⁻¹ K⁻¹. It has anisotropic crystal structure resulting in deterioration of thermoelectric performance in polycrystalline SnSe, providing a low zT of 0.6 and 0.8 for Ag and Na-doped SnSe, respectively. Here, we presented the thermoelectric properties on the K-doped K_xSn_1−xSe (x = 0, 0.1, 0.3, 0.5, 1.5, and 2.0%) polycrystals, synthesized by a high-temperature melting and hot-press sintering with annealing process. The K-doping in SnSe efficiently enhances the hole carrier concentration without significant degradation of carrier mobility. We find that there exist widespread Se-rich precipitates, inducing strong phonon scattering and thus resulting in a very low thermal conductivity. Due to low thermal conductivity and moderate power factor, the K_0.001Sn_0.999Se sample shows an exceptionally high zT of 1.11 at 823 K which is significantly enhanced value in polycrystalline compounds.     

Thermoelectric performance of monolayer Bi2Te2Se of ultra low lattice thermal conductivity

The electronic structure and thermoelectric properties of monolayer Bi₂Te₂Se were studied by density functional theory and semi-classical Boltzmann transport equation. The band gap with TB-mBJ can be improved for monolayer Bi₂Te₂Se. Monolayer Bi₂Te₂Se have ultra-low thermal conductivity comparing with other well-known two-dimensional materials. The monolayer Bi₂Te₂Se can improve electrical conductivities. ZT increases with increasing temperature for monolayer Bi₂Te₂Se. Comparing to GGA, TB-mBJ has larger ZT value in p-type doping. Monolayer Bi₂Te₂Se have larger ZT comparing with other well-known two-dimensional materials. Our calculated results show that our calculation greatly underestimates ZT value, therefore, monolayer Bi₂Te₂Se should have a higher ZT value.     

Understanding the role of defects in influencing the thermoelectric properties of SnSe

As compared to single crystals, polycrystalline SnSe shows a considerable decline in its ZT value. Optimization of carrier concentration by the way of chemical doping is useful but creates point defect and vacancies that are often overlooked. Here we study polycrystalline Sn_0.95M_0.05Se (M = Co, Ni, In) with an aim to understand the role of defects. The overall crystal structure and microstructure of SnSe is not much affected with substitution as evident from X-ray diffraction and scanning electron microscopy study. Rietveld refinement confirms the single phase nature of the all compositions and provides unit cell parameters. Analysis of the stoichiometry reveals the presence of cation vacancies. Optical spectroscopy indicates a degradation of the in-direct gap and Urbach band tail-width fitting confirms the presence of localized states within the gap. Electrical resistivity and Seebeck coefficient are adversely affected by defects, but thermal conductivity decreases by almost 50% of SnSe value.     

Modulation of magnetic properties of bilayer SnSe with transition-metals doping in the interlayer

We investigate the spin-polarized electronic and magnetic properties of bilayer SnSe with transition-metal (TM) atoms doped in the interlayer by using a first-principles method. It shows that Ni dopant cannot induce the magnetism in the doped SnSe sheet, while the ground state of V, Cr, Mn, Fe and Co doped systems are magnetic and the magnetic moment mainly originates from 3d TM atom. Two types of factors, which reduce the magnetic moment of TM atoms doped in bilayer SnSe, are identified as spin-up channel of the 3d orbital loses electrons to SnSe sheet and spin-down channel of the 3d orbital gains electrons from 4s orbital. The spin polarization is found to be 100% at Fermi level for the Mn and Co atoms doped system, while the Ni-doped system is still a semiconductor with a gap of 0.26 eV. These results are potentially useful for development of spintronic devices.     

Enhanced Seebeck effect in graphene devices by strain and doping engineering

In this work, we investigate the possibility of enhancing the thermoelectric power (Seebeck coefficient) in graphene devices by strain and doping engineering. While a local strain can result in the misalignment of Dirac cones of different graphene sections in the k-space, doping engineering leads to their displacement in energy. By combining these two effects, we demonstrate that a conduction gap as large as a few hundred meV can be achieved and hence the enhanced Seebeck coefficient can reach a value higher than 1.4 mV/K in graphene doped heterojunctions with a locally strained area. Such hetero-channels appear to be very promising for enlarging the applications of graphene devices as in strain and thermal sensors.     

Theoretical investigation of the thermoelectric transport properties of BaSi2

The full-potential linear augmented plane wave method based on density functional theory is employed to investigate the electronic structure of BaSi 2 . With the constant relaxation time and rigid band approximation,the electrical conductivity,Seebeck coefficient and figure of merit are calculated by using Boltzmann transport theory,further evaluated as a function of carrier concentration. We find that the Seebeck coefficient is more anisotropic than electrical conductivity. The figure of merit of BaSi 2 is predicted to be quite high at room temperature,implying that optimal doping may be an effective way to improve thermoelectric properties.     

二维MoS2/MoSe2异质材料的电子结构和热电性质研究

利用密度泛函理论结合玻尔兹曼输运理论计算体相和双层二维MoS₂/MoSe₂异质材料的热电性质. 计算表明,体相MoS₂/MoSe₂异质材料的热电性质比之于MoSe₂会有较大程度的提高. 该异质材料热电性质的提高主要源于异质材料本身带隙的减小以及层间的范德瓦尔斯相互作用. 二维MoS₂/MoSe₂异质材料存在热电应用的可能性.     

二维InSe/SnSe2范德华异质结的电子结构和光学特性研究

本文构建了三种不同堆叠形式下的二维InSe/SnSe₂范德华异质结模型,利用基于密度泛函理论的第一性原理方法综合考察了二维InSe/SnSe₂三种不同堆叠情况下的几何构型及稳定性,在此基础上选取具有最稳定性能的构型.该异质结呈现出Ⅱ型能带对齐特征,带隙值为1.118 eV,可以实现电子-空穴的有效分离.另外,相比与单层二维InSe/SnSe₂范德华异质结的光吸收能力达到明显提升,在紫外光范围内吸收系数达到10~6 cm^-1.研究结果将为相关物理实验及机理研究提供理论基础,对二维InSe/SnSe₂范德华异质结在光电器件中的应用具有重要的物理意义.     

基于第一性原理的Mn纳米线掺杂二维SnSe热电性能研究

本文提出了一种在二维SnSe中掺杂一维Mn纳米线的2D-1D复合结构,并系统地研究了其热电性能。结果表明,一维Mn纳米线将电子态汇聚在纳米线附近,提高了材料的各向异性,降低了电子在某一方向上的散射效应,导致了较高的迁移率和电导率。自旋向上和向下的电子态发生简并,导致了较高的塞贝克系数和电导率。此外,Mn纳米线将晶格热导率降低了约0.17 W·m^?1·K^?1。在200至650 K的温度范围内,3Mn-SnSe具有0.73至3.78的极高ZT值,比本征二维SnSe平均提高了约39.2%。     

基于第一性原理的Mn纳米线掺杂二维SnSe热电性能研究

本文提出了一种在二维SnSe中掺杂一维Mn纳米线的2D-1D复合结构,并系统地研究了其热电性能。结果表明,一维Mn纳米线将电子态汇聚在纳米线附近,提高了材料的各向异性,降低了电子在某一方向上的散射效应,导致了较高的迁移率和电导率。自旋向上和向下的电子态发生简并,导致了较高的塞贝克系数和电导率。此外,Mn纳米线将晶格热导率降低了约0.17 W·m^?1·K^?1。在200至650 K的温度范围内,3Mn-SnSe具有0.73至3.78的极高ZT值,比本征二维SnSe平均提高了约39.2%。     

Dynamical stability,electronic and thermoelectric properties of quaternary ZnFeTiSi Heusler compound

We investigated the dynamical stability, electronic and thermoelectric properties of the ZnFeTiSi Heusler compound by combining the first-principles calculations and semi-classical Boltzmann transport theory. The phonon dispersion indicates the dynamical stability and the calculated formation energy is negative which confirm the stability of ZnFeTiSi in the Heusler structure. The calculated electronic structures show that ZnFeTiSi is a semiconductor with an indirect band gap of about 0.573 eV using GGA and 0.643 eV by mBJ-GGA potentials at equilibrium lattice parameter (5.90 Å). Seebeck coefficient, electrical conductivity and electronic thermal conductivity were calculated to describe the thermoelectric properties of the ZnFeTiSi compound. It is found that it exhibits high Seebeck coefficient and power factor, making it promising for future thermoelectric applications.     

Enhanced thermoelectric performance of P-type Sb2Te3 thin films through organic-inorganic hybridization on flexible substrate

In this work, a new idea of organic-inorganic hybridization was proposed to fabricate flexible p-type - Sb₂Te₃/CH₃NH₃I thin films. The CH₃NH₃I has a strong adsorption which can promote the growth of organic molecules, improve the crystallization, and finally increase electrical conductivity. Post-annealing of the fabricated films increased the phonon scattering, thus resulting in a reduction of thermal conductivity and an increased ZT value. The annealed hybrid-composite film showed a significant enhancement in thermoelectric performance, with a maximum ZT value of 0.94 at a temperature of 413 K, which is twice as large as that of the as-deposited film.     

Effective phonon scattering and enhancement of thermoelectric performance in Ga-excess Bi0.4Sb1.6Te3 compounds

We investigate the thermoelectric properties on Ga-excess p-type Ga_xBi_0.4Sb_1.6Te₃ compounds. Even though the random distribution of Ga-doping increases electrical resistivity giving rise to the decrease of power factor, the significant decrease of lattice thermal conductivity by the excess Ga-doping induces significant enhancement of ZT value (1.13 at 350 K) for the Ga x = 0.03 doped compound. From the X-ray diffraction and elemental mapping by energy dispersive X-ray spectroscopy, we observed Sb and Ga phase separation leading to the phonon scattering. The Sb precipitation implies atomic defect in the matrix which can induce short wavelength phonon scattering. The synergetic phonon scatterings from various scattering sources such as point defect, alloy scattering, and grain boundary phonon scattering have an important role in the enhancement of thermoelectric performance.     

Thermoelectric transport coefficients of n-doped CaTiO3, SrTiO3 and BaTiO3: A theoretical study

Boltzmann transport equations and density functional theory calculations were employed to calculate the thermoelectric transport coefficients of CaTiO₃, SrTiO₃ and BaTiO₃. It was found that BaTiO₃ has the largest Seebeck coefficient and power factor. Then the transport coefficients were analyzed using the ‘Tight Binding Model’. The band narrowing, caused by the increasing lattice constants from CaTiO₃ to BaTiO₃, was the main reason for the increasing Seebeck coefficients and the decreasing electrical conductivity. The calculated electrical conductivity and electronic thermal conductivity were in line with the Wiedemann-Franz law and the Lorenz factor was determined to be 2.45 for these oxides as degenerate semiconductors. Our theoretical results are helpful for seeking high performance thermoelectric oxides.     

Electronic and thermoelectric properties of Mg_2Ge_xSn-_(1-x)(x=0.25,0.50,0.75) solid solutions by first-principles calculations

The electronic structure and thermoelectric(TE) properties of Mg_2Ge_xSn_(1-x)(x = 0.25, 0.50, 0.75) solid solutions are investigated by first-principles calculations and semi-classical Boltzmann theory. The special quasi-random structure(SQS) is used to model the solid solutions, which can produce reasonable band gaps with respect to experimental results.The n-type solid solutions have an excellent thermoelectric performance with maximum zT values exceeding 2.0, where the combination of low lattice thermal conductivity and high power factor(PF) plays an important role. These values are higher than those of pure Mg_2Sn and Mg_2Ge. The p-type solid solutions are inferior to the n-type ones, mainly due to the much lower PF. The maximum zT value of 0.62 is predicted for p-type Mg_2Ge_(0.25)Sn_(0.75) at 800K. The results suggest that the n-type Mg_2Ge_xSn_(1-x) solid solutions are promising mid-temperature TE materials.