We study theoretically the effects of anisotropy on the thermoelectric performance of $p$-type AgBiSe$_2$. We present an apparent realization of the thermoelectric benefits of one-dimensional "plate-like" carrier pocket anisotropy in the valence band of this material. Based on first principles calculations we find a substantial anisotropy in the electronic structure, likely favorable for thermoelectric performance, in the valence bands of the hexagonal phase of the silver chalcogenide thermoelectric AgBiSe$_2$, while the conduction bands are more isotropic, and in our experiments do not attain high performance. AgBiSe$_2$ has already exhibited a $ZT$ value of 1.5 in a high-temperature disordered fcc phase, but room-temperature performance has not been demonstrated. We develop a theory for the ability of anisotropy to decouple the density-of-states and conductivity effective masses, pointing out the influence of this effect in the high performance thermoelectrics Bi$_2$Te$_3$ and PbTe. From our first principles and Boltzmann transport calculations we estimate the performance of $p$-type AgBiSe$_{2}$.
We report first-principles density-functional study of electron-phonon interactions and thermoelectric transport properties of full-Heusler compounds Sr$_{2}$BiAu and Sr$_{2}$SbAu. Our results show that ultrahigh intrinsic bulk thermoelectric performance across a wide range of temperatures is physically possible and point to the presence of multiply degenerate and highly dispersive carrier pockets as the key factor for achieving it. Sr$_{2}$BiAu, which features ten energy-aligned low effective mass pockets (six along $Γ-X$ and four at $L$), is predicted to deliver $n$-type $zT=0.4-4.9$ at $T=1…
We present a study of angle-resolved quantum oscillations of electric and thermoelectric transport coefficients in semi-metallic WTe$_{2}$, which has the particularity of displaying a large B$^{2}$ magneto-resistance. The Fermi surface consists of two pairs of electron-like and hole-like pockets of equal volumes in a "Russian doll" structure. Carrier density, Fermi energy, mobility and the mean-free-path of the system are quantified. An additional frequency is observed above a threshold field and attributed to magnetic breakdown across two orbits. In contrast to all other dilute metals, the Ne…
Heusler type compounds have long been recognized as potential thermoelectric (TE) materials. Here, the experimentally observed TE properties of Fe$_{2}$VAl are understood through electronic structure calculations in the temperature range of $300-800$ K. The observed value of $S$ is $\sim-$138 $μ$V/K at 300 K. Then, the $|S|$ decreases with increase in temperature up to the highest temperature with the value of $\sim-$18 $μ$V/K at 800 K. The negative sign of $S$ in the full temperature window signifies the dominating $n$-type character of the compound. The temperature dependent of electrical co…
Lifshitz transition, a change in Fermi surface topology, is likely to greatly influence exotic correlated phenomena in solids, such as high-temperature superconductivity and complex magnetism. However, since the observation of Fermi surfaces is generally difficult in the strongly correlated systems, a direct link between the Lifshitz transition and quantum phenomena has been elusive so far. Here, we report a marked impact of the pressure-induced Lifshitz transition on thermoelectric performance for SnSe, a promising thermoelectric material without strong electron correlation. By applying press…
Using first-principles density-functional theory calculations, we predict the potential for unprecedented thermoelectric efficiency $zT=5$ at 800 K in $n$-type Ba$_{2}$BiAu full-Heusler compound. Such a high efficiency arises from an intrinsically ultralow lattice thermal conductivity coupled with a very high power factor reaching 7 mW m$^{-1}$ K$^{-2}$ at 500 K. The high power factor originates from a light, sixfold degenerate conduction band pocket along the $Γ$-X direction. Weak acoustic phonon scattering and sixfold multiplicity combine to yield high mobility and high Seebeck coefficient. …
Here, we study the thermoelectric properties of topological semimetal CoSi in the temperature range $300-800$ K by using combined experimental and density functional theory (DFT) based methods. CoSi is synthesized using arc melting technique and the Rietveld refinement gives the lattice parameters of a = b = c = 4.445 Å. The measured values of Seebeck coefficient (S) shows the non-monotonic behaviour in the studied temperature range with the value of $\sim-$81 $μ$V/K at room temperature. The $|S|$ first increases till 560 K ($\sim-$93 $μ$V/K) and then decreases up to 800 K ($\sim-$84 $μ$V/K) i…
Using first principles calculations, we study the conduction band alignment, effective mass, and Fermi surface complexity factor of n-type Mg3Sb2-xBix (x = 0, 1, and 2) from the full ab initio band structure. We find that with increasing the Bi content the K and M band minima moves away from the conduction band minimum CB1 while the singly-degenerate $Γ$ band minimum shifts rapidly downward and approaches the conduction band minimum. But the favorable six-fold degenerate CB1 band minimum keeps dominating the conduction band minimum and there is no band crossing between the $Γ$ and CB1 band min…
Understanding how to optimize electronic band structures for thermoelectrics is a topic of long-standing interest in the community. Prior models have been limited to simplified bands and/or scattering models. In this study, we apply more rigorous scattering treatments to more realistic model band structures - upward-parabolic bands that inflect to an inverted parabolic behavior - including cases of multiple bands. In contrast to common descriptors (e.g., quality factor and complexity factor), the degree to which multiple pockets improve thermoelectric performance is bounded by interband scatte…
We report on low-energy electronic structure and electronic correlations of K$_{0.65}$RhO$_2$, studied using high-resolution angle-resolved photoemission spectroscopy (ARPES) technique and density functional theory (DFT) calculations. We observe a highly correlated hole pocket on the Fermi surface. We further notice that the correlations are momentum dependent. Most importantly, two $kinks$ at binding energies of 75 meV and 195 meV have been observed from the band dispersion in the vicinity of the Fermi level. While the low energy $kink$ at 75 meV can be understood as a result of the electron-…
PbTe is a leading mid-range thermoelectric material with a $zT$ that has been enhanced by, amongst other methods, band engineering. Here we present an experimental study of the Hall effect, quantum oscillations, specific heat, and electron microprobe analysis that explores the evolution of the electronic structure of PbTe heavily doped with the `ideal' acceptor Na up to the solubility limit. We identify two phenomenological changes that onset as the electronic structure deviates from a Kane-type dispersion at around 180meV; a qualitative change in the field dependence of the Hall effect indica…
We performed the angle dependent magnetoresistance (MR), Hall effect measurements, the temperature dependent magneto-thermoelectric power (TEP) S(T) measurements, and the first-principles calculations to study the electronic properties of orthorhombic phase MoTe2 (Td-MoTe2), which was proposed to be electronically two-dimensional (2D). There are some interesting findings about Td-MoTe2: (1) A scaling approach εθ=(sin2θ+γ-2cos2θ)1/2 is applied, where θ is the magnetic field angle with respect to the c axis of the crystal and γ is the mass anisotropy. Unexpectedly, the electronically 3D characte…
