Thermoelectric prospects of nanomaterials with spin-orbit surface bands

Nanostructured composites and nanowire arrays of traditional thermoelectrics like Bi, Bi(1-x)Sb(x) and Bi(2)Te(3) have metallic Rashba surface spin-orbit bands featuring high mobilities rivaling that of the bulk for which topological insulator behavior has been proposed. Nearly pure surface electronic transport has been observed at low temperatures in Bi nanowires with diameter around the critical diameter, 50 nm, for the semimetal-to semiconductor transition. The surface contributes strongly to the thermopower, actually dominating for temperatures T < 100 K in these nanowires. The surface thermopower was found to be -1 T microvolt/(K^2), a value that is consistent with theory. We show that surface electronic transport together with boundary phonon scattering leads to enhanced thermoelectric performance at low temperatures of Bi nanowire arrays. We compare with bulk n-BiSb alloys, optimized CsBi(4)Te(6) and optimized Bi(2)Te(3). Surface dominated electronic transport can be expected in nanomaterials of the other traditional thermoelectrics.Comment: 18 pages, 3 figure

Thermoelectric properties of the bismuth telluride nanowires in the constant-relaxation-time approximation

Electronic structure of bismuth telluride nanowires with the growth directions [110] and [015] is studied in the framework of anisotropic effective mass method using the parabolic band approximation. The components of the electron and hole effective mass tensor for six valleys are calculated for both growth directions. For a square nanowire, in the temperature range from 77 K to 500 K, the dependence of the Seebeck coefficient, the electron thermal and electrical conductivity as well as the figure of merit ZT on the nanowire thickness and on the excess hole concentration are investigated in the constant-relaxation-time approximation. The carrier confinement is shown to play essential role for square nanowires with thickness less than 30 nm. The confinement decreases both the carrier concentration and the thermal conductivity but increases the maximum value of Seebeck coefficient in contrast to the excess holes (impurities). The confinement effect is stronger for the direction [015] than for the direction [110] due to the carrier mass difference for these directions. The carrier confinement increases maximum value of ZT and shifts it towards high temperatures. For the p-type bismuth telluride nanowires with growth direction [110], the maximum value of the figure of merit is equal to 1.3, 1.6, and 2.8, correspondingly, at temperatures 310 K, 390 K, 480 K and the nanowire thicknesses 30 nm, 15 nm, and 7 nm. At the room temperature, the figure of merit equals 1.2, 1.3, and 1.7, respectively.Comment: 13 pages, 7 figures, 2 tables, typos added, added references for sections 2-

Pressure effects on the transport coefficients of Ba(Fe1-xCox)2As2

We report the temperature dependence of the resistivity and thermoelectric power under hydrostatic pressure of the itinerant antiferromagnet BaFe2As2 and the electron-doped superconductor Ba(Fe0.9Co0.1)2As2. We observe a hole-like contribution to the thermopower below the structural-magnetic transition in the parent compound that is suppressed in magnitude and temperature with pressure. Pressure increases the contribution of electrons to transport in both the doped and undoped compound. In the 10% Co-doped sample, we used a two-band model for thermopower to estimate the carrier concentrations and determine the effect of pressure on the band structure

Thermoelectric Figure of Merit of Strongly Correlated Superlattice Semiconductors

We solved the Anderson Lattice Hamiltonian to get the energy bands of a strongly correlated semiconductor by using slave boson mean field theory. The transport properties were calculated in the relaxation-time approximation,and the thermoelectric figure of merit was obtained for the strongly correlated semiconductor and its superlattice structures. We found that at room temperature $ZT$ can reach nearly 2 for the quantum wire lattice structure.We believe that it is possible to find high values of thermoelectric figure of merit from strongly correlated semiconductor superlattice systems.Comment: 4 pages, 3 figure

A simple model for the vibrational modes in honeycomb lattices

The classical lattice dynamics of honeycomb lattices is studied in the harmonic approximation. Interactions between nearest neighbors are represented by springs connecting them. A short and necessary introduction of the lattice structure is presented. The dynamical matrix of the vibrational modes is then derived, and its eigenvalue problem is solved analytically. The solution may provide deeper insight into the nature of the vibrational modes. Numerical results for the vibrational frequencies are presented. To show that how effective our method used for the case of honeycomb lattice is, we also apply it to triangular and square lattice structures. A few suggested problems are listed in the concluding section.Comment: 9 pages, 12 figures, submitted to American Journal of Physic

Pressure-induced phase transition of Bi2Te3 into the bcc structure

The pressure-induced phase transition of bismuth telluride, Bi2Te3, has been studied by synchrotron x-ray diffraction measurements at room temperature using a diamond-anvil cell (DAC) with loading pressures up to 29.8 GPa. We found a high-pressure body-centered cubic (bcc) phase in Bi2Te3 at 25.2 GPa, which is denoted as phase IV, and this phase apperars above 14.5 GPa. Upon releasing the pressure from 29.8 GPa, the diffraction pattern changes with pressure hysteresis. The original rhombohedral phase is recovered at 2.43 GPa. The bcc structure can explain the phase IV peaks. We assumed that the structural model of phase IV is analogous to a substitutional binary alloy; the Bi and Te atoms are distributed in the bcc-lattice sites with space group Im-3m. The results of Rietveld analysis based on this model agree well with both the experimental data and calculated results. Therefore, the structure of phase IV in Bi2Te3 can be explained by a solid solution with a bcc lattice in the Bi-Te (60 atomic% tellurium) binary system.Comment: 12 pages, 5 figure

Giant Anharmonic Phonon Scattering in PbTe

Understanding the microscopic processes affecting the bulk thermal conductivity is crucial to develop more efficient thermoelectric materials. PbTe is currently one of the leading thermoelectric materials, largely thanks to its low thermal conductivity. However, the origin of this low thermal conductivity in a simple rocksalt structure has so far been elusive. Using a combination of inelastic neutron scattering measurements and first-principles computations of the phonons, we identify a strong anharmonic coupling between the ferroelectric transverse optic (TO) mode and the longitudinal acoustic (LA) modes in PbTe. This interaction extends over a large portion of reciprocal space, and directly affects the heat-carrying LA phonons. The LA-TO anharmonic coupling is likely to play a central role in explaining the low thermal conductivity of PbTe. The present results provide a microscopic picture of why many good thermoelectric materials are found near a lattice instability of the ferroelectric type

An efficient algorithm to calculate intrinsic thermoelectric parameters based on Landauer approach

The Landauer approach provides a conceptually simple way to calculate the intrinsic thermoelectric (TE) parameters of materials from the ballistic to the diffusive transport regime. This method relies on the calculation of the number of propagating modes and the scattering rate for each mode. The modes are calculated from the energy dispersion (E(k)) of the materials which require heavy computation and often supply energy relation on sparse momentum (k) grids. Here an efficient method to calculate the distribution of modes (DOM) from a given E(k) relationship is presented. The main features of this algorithm are, (i) its ability to work on sparse dispersion data, and (ii) creation of an energy grid for the DOM that is almost independent of the dispersion data therefore allowing for efficient and fast calculation of TE parameters. The inclusion of scattering effects is also straight forward. The effect of k-grid sparsity on the compute time for DOM and on the sensitivity of the calculated TE results are provided. The algorithm calculates the TE parameters within 5% accuracy when the K-grid sparsity is increased up to 60% for all the dimensions (3D, 2D and 1D). The time taken for the DOM calculation is strongly influenced by the transverse K density (K perpendicular to transport direction) but is almost independent of the transport K density (along the transport direction). The DOM and TE results from the algorithm are bench-marked with, (i) analytical calculations for parabolic bands, and (ii) realistic electronic and phonon results for $Bi_{2}Te_{3}$.Comment: 16 Figures, 3 Tables, submitted to Journal of Computational electronic

Glass-Like Heat Conduction in High-Mobility Crystalline Semiconductors

The thermal conductivity of polycrystalline semiconductors with type-I clathrate hydrate crystal structure is reported. Ge clathrates (doped with Sr and/or Eu) exhibit lattice thermal conductivities typical of amorphous materials. Remarkably, this behavior occurs in spite of the well-defined crystalline structure and relatively high electron mobility ($\sim 100 cm^2/Vs$). The dynamics of dopant ions and their interaction with the polyhedral cages of the structure are a likely source of the strong phonon scattering.Comment: 4 pages, 3 postscript figures, to be published, Phys. Rev. Let