We propose a possible route to achieve high thermoelectric efficiency in molecular junctions by combining a local chemical tuning of the molecular electronic states with the use of semiconducting electrodes. The former allows to control the position of the HOMO transmission resonance with respect to the Fermi energy while the latter fulfills a twofold purpose: the suppression of electron-like contributions to the thermopower and the cut-off of the HOMO transmission tails into the semiconductor band gap. As a result a large thermopower can be obtained. Our results strongly suggest that large figures of merit in such molecular junctions can be achieved.
Thermoelectrics are promising by directly generating electricity from waste heat. However, (sub-)room-temperature thermoelectrics have been a long-standing challenge due to vanishing electronic entropy at low temperatures. Topological materials offer a new avenue for energy harvesting applications. Recent theories predicted that topological semimetals at the quantum limit can lead to a large, non-saturating thermopower and a quantized thermoelectric Hall conductivity approaching a universal value. Here, we experimentally demonstrate the non-saturating thermopower and quantized thermoelectric H…
Weyl semimetals combine topological and semimetallic effects, making them candidates for interesting and effective thermoelectric transport properties. Here, we present experimental results on polycrystalline NbP, demonstrating the simultaneous existence of a large Nernst effect and a large magneto-Seebeck effect, which is typically not observed in a single material at the same temperature. We compare transport results from two polycrystalline samples of NbP with previously published work, observing a shift in the temperature at which the maximum Nernst and magneto-Seebeck thermopowers occur, …
We predict high thermoelectric efficiency in the layered perovskite La$_2$Ti$_2$O$_7$, based on calculations (mostly ab-initio) of the electronic structure, transport coefficients, and thermal conductivity in a wide temperature range. The figure of merit $ZT$ computed with a temperature-dependent relaxation time increases monotonically from just above 1 at room temperature to over 2.5 at 1200 K, at an optimal carrier density of around 10$^{20}$ cm$^{-3}$. The Seebeck thermopower coefficient is between 200 and 300 $μ$V/K at optimal doping, but can reach nearly 1 mV/K at low doping. Much of the …
We report on thermoelectric properties of nanocrystalline Cr$_{\rm 1-x}$Si$_{\rm x}$ composite films. As-deposited amorphous films were transformed into a nanocrystalline state with average grain size of 10--20~nm by annealing during in-situ thermopower and electrical resistivity measurements. The partially crystallized films, i.e. the films consisting of crystalline grains dispersed in the amorphous matrix, are a new type of the heterogeneous material where the nanocrystalline phase plays the role of scattering centers giving rise to a large contribution to the thermopower. We show that the t…
An unconventional approach to enhance the transverse thermopower by combining magnetic and thermoelectric materials, namely the Seebeck-driven transverse thermoelectric generation (STTG), has been proposed and demonstrated recently. Here, we improve on the previously used sample structure and achieve large transverse thermopower over 40 $μ$V K$^{-1}$ due to STTG in on-chip devices. We deposited polycrystalline Fe-Ga alloy films directly on n-type Si substrates, where Fe-Ga and Si serve as the magnetic and thermoelectric materials, respectively. Using microfabrication, contact holes were create…
We present here the thermoelectric properties of olivine-type Fe2GeCh4 (Ch = S, Se and Te) using the linear augmented plane wave method based on first principles density functional calculations. The calculated transport properties using the semi-local Boltzmann transport equation reveal very high thermopower for both S and Se-based compounds compared to their Te counterparts. The main reason for this high thermopower is the quasi-flat nature of the bands at the valence and conduction band edges. The calculated thermopower of Fe2GeCh4 is in good agreement with the experimental reports at room t…
Confined electrons in low dimensions host desirable material functions for downscaled electronics as well as advanced energy technologies. Thermoelectricity is a most fascinating example, since the dimensionality modifies the electron density of states dramatically, leading to enhanced thermopower as experimentally examined in artificial two-dimensional (2D) structures. However, it is still an open question whether such an enhanced thermopower in low dimensions is realized in layered materials with strong 2D characters such as cuprates. Here, we report unusual enhancement of the thermopower in…
Na-site substitution effects of the thermoelectric properties of NaCo_2O_4
测量并分析了Na $_{1+x}$ Co $_2$ O $_4$和Na $_{1.1-x}$ Ca $_x$ Co $_2$ O $_4$的电阻率和热电势。在Na $_{1+x}$ Co $_2$ O $_4$中，电阻率随$x$增加，而热电势几乎与$x$无关。这表明过量的Na不太可能提供载流子，并且减少了样品中的有效导电路径。在Na $_{1.1-x}$ Ca $_x$ Co $_2$ O $_4$中，电阻率和热电势随着$x$而增加，并且Ca $^{2+}$取代Na $^+$减少了NaCo $_2$ O $_4$中的多数载流子。这意味着它们是孔，这与热电势的正号一致。该化合物的电阻率随温度变化的特性证明了该化合物具有很强的相关性。
In this paper we explore the different mechanisms that affect the thermopower of a band insulating perovskite (in this case, SrTiO$_3$) when subject to strain (both compressive or tensile). We analyze the high temperature, entropy dominated limit and the lower temperature, energy-transport regime. We observe that the effect of strain in the high-temperature Seebeck coefficient is small at the concentration levels of interest for thermoelectric applications. However, the effective mass changes substantially with strain, which produces an opposite effect to that of the degeneracy-breakups produc…
The Seebeck-driven transverse thermoelectric generation in magnetic/thermoelectric hybrid materials (STTG) has been investigated in all-bulk hybrid materials. The transverse thermopower in a ferromagnetic Co$_2$MnGa/thermoelectric $n$-type Si hybrid bulk material with the adjusted dimensions reaches 16.0 $μ$V/K at room temperature with the aid of the STTG contribution, which is much larger than the anomalous Nernst coefficient of the Co$_2$MnGa slab (6.8 $μ$V/K). Although this transverse thermopower is smaller than the value for previously reported thin-film-based hybrid materials, the hybrid …
We investigated the effect of pressure on the magnetic and thermoelectric properties of Sr$_{3.1}$Y$_{0.9}$Co$_{4}$O$_{10+δ}$. The magnetization is reduced with the application of pressure, reflecting the spin-state modification of the Co$^{3+}$ ions into the nonmagnetic low-spin state. Accordingly, with increasing pressure, the Seebeck coefficient is enhanced, especially at low temperatures, at which the effect of pressure on the spin state becomes significant. These results indicate that the spin-orbital entropy is a key valuable for the thermoelectric properties of the strongly correlated c…
We present a fully ab initio based scheme to compute transport properties, i.e. the electrical conductivity σ and thermopower S, in the presence of electron-phonon interaction. Therefore, we explicitly investigate the k-dependent structure of the Eliashberg spectral function , the coupling strength, the linewidth and the relaxation time τ. We obtain a state-dependent τ and show its necessity to reproduce the increased thermopower at temperatures below the Debye temperature, without accounting for the phonon-drag effect. Despite the detailed investigations of various k and q dependencies, the p…
We have measured the electrical resistivity and the thermopower of the electron-doped perovskite cobaltites LaCo$_{1-y}$Te$_y$O$_3$. In contrast to the hole-doped systems such as metallic ferromagnets La$_{1-x}M_x$CoO$_3$ ($M$ = Ca, Sr, Ba), the electron-doped samples show an insulating behavior even in a heavily doped range due to a spin-state blockade mechanism that an electron hopping from high-spin Co$^{2+}$ to low-spin Co$^{3+}$ site is energetically suppressed. We find that, despite the electron doping, the thermopower shows relatively large positive values above $y=0.05$, strikingly dis…
Transverse thermoelectric devices produce electric fields perpendicular to an incident heat flux. Classically, this process is driven by the Nernst effect in bulk solids, wherein a magnetic field generates a Lorentz force on thermally excited electrons. The spin Seebeck effect (SSE) also produces magnetization-dependent transverse electric fields. SSE is traditionally observed in thin metallic films deposited on electrically insulating ferromagnets, but the films' high resistance limits thermoelectric conversion efficiency. Combining Nernst and SSE in bulk materials would enable devices with s…
The search for new thermoelectric materials aims at improving their power and efficiency, as expressed by thermopower $S$ and figure of merit $ZT$. By considering a very general transport spectral function $W(E)$, expressions for $S$ and $ZT$ can be derived, which contain the statistical weights of an effective distribution function only, see Refs. \cite{eltschka16,mahan96,matveev00}. We assumption of a Lorentzian shape with width $k_BT$ resulting from the electron-phonon coupling allows to estimate an upper limit of $S$ and $ZT$ independent on the microscopic mechanisms of the transport proce…
Interest in the application of thermoelectric devices for renewable energy has risen over the past decade. In this paper, we calculate the transport properties of various configurations of the transition metal dichalcogenide (TMD) MSe$_2$ (M = Hf, Zr, Ti) in search of promising thermoelectric materials at low/high temperatures. We explore the properties of the pure monolayer at discrete levels of biaxial tensile strain (epsilon = 0%, 2%, 4%, 8%), as well as those of the van der Waals heterobilayers MSe$_2$/MSe$_2$ using first-principles calculations combined with semi-classical Boltzmann trans…
Influence of strain on anisotropic thermoelectric transport of Bi$_2$Te$_3$ and Sb$_2$Te$_3$
基于详细的第一性原理计算和半经典Boltzmann输运理论，研究了应变下Bi $_2$ Te $_3$和Sb $_2$ Te $_3$的各向异性热电输运性质.发现由于应变相关的热电势和电导率的补偿效应，Bi $_2$ Te $_3, while being stable for Sb$ _2 $Te$ _3 $. A clear preference for thermoelectric transport under hole-doping, as well as for the in-plane transport direction was found for both tellurides. In contrast to the electrical conductivity anisotropy, the anisotropy of the thermopower was almost robust under applied strain. The assumption of an anisotropic relaxation time for Bi$ _2 $Te$ _3在面内应变下，相关的功率因数将降低。这表明，在单晶系统中，强的各向异性散射效应已经起作用。
We present first room-temperature thermoelectric signature of the skyrmion lattice. This was observed in Fe3Sn2, a Kagome Dirac crystal with massive Dirac fermions that features high-temperature skyrmion phase. The room-temperature skyrmion lattice shows magnetic-field dependence of the wavevector whereas thermopower is dominated by the electronic diffusion mechanism, allowing for the skyrmionic bubble lattice detection. Our results pave the way for the future skyrmion-based devices based on the manipulation of the thermal gradient.
p x n-type materials refer to materials with a p-type Seebeck coefficient in one direction and a n-type coefficient in the orthogonal direction. This type of materials allows for a transverse thermoelectric response, which is highly desirable for energy applications. Here, we report the observation of p x n-type behavior in TaIrTe4, a type-II Weyl semimetal, with an in-plane thermopower anisotropy S$_{xx}$-S$_{yy}$ reaches a maximum value 40$μ$V/K at 200K. Intriguingly. we found that such a p x n-type behavior is absent in the similar compound NbIrTe4. The presence and absence of p x n-type be…
Thermal fluctuation of local magnetization in magnetic metals intercoupled with charge carriers and phonons offers a path to enhance thermoelectric performance. The thermopower enhancement by spin fluctuations (SF) has been observed before. However, the crucial evidence for enhancing thermoelectric-figure-of-merit (zT) by SF has not been reported until now. Here we report evidence for such enhancement in the ferromagnetic CrTe. The SF leads to nearly 80% zT enhancement in ferromagnetic CrTe near and below TC~335 K. The ferromagnetism in CrTe is originated from the collective electronic and loc…
Short-range magnetic correlations can significantly increase the thermopower of magnetic semiconductors, representing a noteworthy development in the decades-long effort to develop high-performance thermoelectric materials. Here, we reveal the nature of the thermopower-enhancing magnetic correlations in the antiferromagnetic semiconductor MnTe. Using magnetic pair distribution function analysis of neutron scattering data, we obtain a detailed, real-space view of robust, nanometer-scale, antiferromagnetic correlations that persist into the paramagnetic phase above the Néel temperature $T_{\math…
