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Showing papers on "Seebeck coefficient published in 2016"


Journal ArticleDOI
08 Jan 2016-Science
TL;DR: A record high ZTdev ∼1.34, with ZT ranging from 0.7 to 2.0 at 300 to 773 kelvin, realized in hole-doped tin selenide (SnSe) crystals, arises from the ultrahigh power factor, which comes from a high electrical conductivity and a strongly enhanced Seebeck coefficient enabled by the contribution of multiple electronic valence bands present in SnSe.
Abstract: Thermoelectric technology, harvesting electric power directly from heat, is a promising environmentally friendly means of energy savings and power generation. The thermoelectric efficiency is determined by the device dimensionless figure of merit ZT(dev), and optimizing this efficiency requires maximizing ZT values over a broad temperature range. Here, we report a record high ZT(dev) ∼1.34, with ZT ranging from 0.7 to 2.0 at 300 to 773 kelvin, realized in hole-doped tin selenide (SnSe) crystals. The exceptional performance arises from the ultrahigh power factor, which comes from a high electrical conductivity and a strongly enhanced Seebeck coefficient enabled by the contribution of multiple electronic valence bands present in SnSe. SnSe is a robust thermoelectric candidate for energy conversion applications in the low and moderate temperature range.

1,542 citations


Journal ArticleDOI
TL;DR: In this paper, the physical and chemical properties of various thermoelectric materials are reviewed and strategies for improving the performance of materials are proposed, along with an insight into semiconductor physics.

499 citations


Journal ArticleDOI
TL;DR: The deceptively simple material SnSe has surprised the scientific community by showing an unexpectedly low thermal conductivity and high power factor and it has become a very promising thermoelectric material as discussed by the authors.
Abstract: The deceptively simple material SnSe has surprised the scientific community by showing an unexpectedly low thermal conductivity and high power factor and it has become a very promising thermoelectric material. Both the electrical and thermal transport properties of SnSe are outstanding. It is remarkable that a binary compound exhibits strong anharmonic and anisotropic bonding, and after hole doping it shows an exceptionally high power factor because of a high electrical conductivity and a strongly enhanced Seebeck coefficient. The latter is enabled by the contribution of multiple electronic valence bands. In this perspective, we discuss the natural features of SnSe, including crystal structures, electronic band structures, and physical and chemical properties. We also compare the electrical transport properties of single crystals and polycrystalline SnSe. The thermal conductivities of polycrystalline samples show wide variation from laboratory to laboratory, with some values being higher than those of single crystals and some lower, which has caused confusion and controversy. To address the issues regarding the thermal transport properties of SnSe, we systematically summarize the reports for SnSe variants, discuss them along with some of our own new results, and offer possible explanations. Finally, some possible strategies are proposed toward future enhancements of the thermoelectric figure of merit of SnSe.

391 citations


Journal ArticleDOI
TL;DR: In this paper, the authors summarise the recent progress in bulk thermoelectric (TE) materials and summarize the recently achieved enhancements in the TE performance encompassing the use of electronic band structure engineering, lattice phon...
Abstract: Thermoelectric (TE) materials facilitate direct heat-to-electricity conversion. The performance of a TE material is characterised by its figure of merit zT (=S2 σT/κ) that depends on both electronic transport properties, i.e. the Seebeck coefficient S and the electrical conductivity σ, and on thermal transport properties, i.e. the thermal conductivity κ of a material. The intrinsically counter-correlated behaviour between electronic and thermal transport properties makes the enhancement of zT a very challenging task. In the past 10 years, the zTs in bulk TE materials have been significantly enhanced due to intensive exploratory efforts, the discovery of new physical phenomena and effects, and applications of advanced synthesis methods. In this review, we summarise the recent progress in bulk TE materials. After the introduction of fundamental principles of thermoelectricity, the recently achieved enhancements in the TE performance encompassing the use of electronic band structure engineering, lattice phon...

380 citations


Journal ArticleDOI
TL;DR: The average value of the figure of merit ZT, of more than 1.17, is measured from 300 K to 800 K along the crystallographic b-axis of 3 at% Na-doped SnSe, with the maximum ZT reaching a value of 2 at 800 K as mentioned in this paper.
Abstract: Excellent thermoelectric performance is obtained over a broad temperature range from 300 K to 800 K by doping single crystals of SnSe. The average value of the figure of merit ZT, of more than 1.17, is measured from 300 K to 800 K along the crystallographic b-axis of 3 at% Na-doped SnSe, with the maximum ZT reaching a value of 2 at 800 K. The room temperature value of the power factor for the same sample and in the same direction is 2.8 mW mK−2, which is an order of magnitude higher than that of the undoped crystal. Calculations show that Na doping lowers the Fermi level and increases the number of carrier pockets in SnSe, leading to a collaborative optimization of the Seebeck coefficient and the electrical conductivity. The resultant optimized carrier concentration and the increased number of carrier pockets near the Fermi level in Na-doped samples are believed to be the key factors behind the spectacular enhancement of the average ZT.

372 citations


Journal ArticleDOI
TL;DR: Using the Te-PEDOT:PSS hybrid composites, a flexible thermoelectric generator that could be embedded in textiles was fabricated by a printing process and generates a thermoeLECTric voltage of 2 mV using human body heat.
Abstract: The thermoelectric properties of poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) and tellurium-PEDOT:PSS (Te-PEDOT:PSS) hybrid composites were enhanced via simple chemical treatment. The performance of thermoelectric materials is determined by their electrical conductivity, thermal conductivity and Seebeck coefficient. Significant enhancement of the electrical conductivity of PEDOT:PSS and Te-PEDOT:PSS hybrid composites from 787.99 and 11.01 to 4839.92 and 334.68 S cm−1, respectively was achieved by simple chemical treatment with H2SO4. The power factor of the developed materials could be effectively tuned over a very wide range depending on the concentration of the H2SO4 solution used in the chemical treatment. The power factors of the developed thermoelectric materials were optimized to 51.85 and 284 μW m−1 K−2, respectively, which represent an increase of four orders of magnitude relative to the corresponding parameters of the untreated thermoelectric materials. Using the Te-PEDOT:PSS hybrid composites, a flexible thermoelectric generator that could be embedded in textiles was fabricated by a printing process. This thermoelectric array generates a thermoelectric voltage of 2 mV using human body heat.

315 citations


Journal ArticleDOI
TL;DR: This work systematically investigated the thermoelectric properties of polycrystalline SnSe doped with three alkali metals (Li, Na, and K) and found that Na has the best doping efficiency.
Abstract: Recent findings about ultrahigh thermoelectric performance in SnSe single crystals have stimulated related research on this simple binary compound, which is focused mostly on its polycrystalline counterparts, and particularly on electrical property enhancement by effective doping. This work systematically investigated the thermoelectric properties of polycrystalline SnSe doped with three alkali metals (Li, Na, and K). It is found that Na has the best doping efficiency, leading to an increase in hole concentration from 3.2 × 10(17) to 4.4 × 10(19) cm(-3) at room temperature, accompanied by a drop in Seebeck coefficient from 480 to 142 μV/K. An equivalent single parabolic band model was found adequate to capture the variation tendency of Seebeck coefficient with doping levels within a wide range. A mixed scattering of carriers by acoustic phonons and grain boundaries is suitable for numerically understanding the temperature-dependence of carrier mobility. A maximum ZT of ∼0.8 was achieved in 1% Na- or K-doped SnSe at 800 K. Possible strategies to improve the mobility and ZT of polycrystals were also proposed.

270 citations


Journal ArticleDOI
TL;DR: In this article, the ionic thermoelectric supercapacitor (ITESC) is charged under a temperature gradient, and the stored electrical energy can be delivered to an external circuit.
Abstract: Temperature gradients are generated by the sun and a vast array of technologies and can induce molecular concentration gradients in solutions via thermodiffusion (Soret effect). For ions, this leads to a thermovoltage that is determined by the thermal gradient ΔT across the electrolyte, together with the ionic Seebeck coefficient αi. So far, redox-free electrolytes have been poorly explored in thermoelectric applications due to a lack of strategies to harvest the energy from the Soret effect. Here, we report the conversion of heat into stored charge via a remarkably strong ionic Soret effect in a polymeric electrolyte (Seebeck coefficients as high as αi = 10 mV K−1). The ionic thermoelectric supercapacitor (ITESC) is charged under a temperature gradient. After the temperature gradient is removed, the stored electrical energy can be delivered to an external circuit. This new means to harvest energy is particularly suitable for intermittent heat sources like the sun. We show that the stored electrical energy of the ITESC is proportional to (ΔTαi)2. The resulting ITESC can convert and store several thousand times more energy compared with a traditional thermoelectric generator connected in series with a supercapacitor.

268 citations


Journal ArticleDOI
TL;DR: enhanced thermoelectric performance in SnTe, where significantly improved electrical transport properties and reduced thermal conductivity were achieved simultaneously are reported, suggesting that SnTe is a robust candidate for medium-temperature thermoelectedric applications.
Abstract: We report enhanced thermoelectric performance in SnTe, where significantly improved electrical transport properties and reduced thermal conductivity were achieved simultaneously. The former was obtained from a larger hole Seebeck coefficient through Fermi level tuning by optimizing the carrier concentration with Ga, In, Bi, and Sb dopants, resulting in a power factor of 21 μW cm(-1) K(-2) and ZT of 0.9 at 823 K in Sn(0.97)Bi(0.03)Te. To reduce the lattice thermal conductivity without deteriorating the hole carrier mobility in Sn(0.97)Bi(0.03)Te, SrTe was chosen as the second phase to create strained endotaxial nanostructures as phonon scattering centers. As a result, the lattice thermal conductivity decreases strongly from ∼2.0 Wm(-1) K(-1) for Sn(0.97)Bi(0.03)Te to ∼1.2 Wm(-1) K(-1) as the SrTe content is increased from 0 to 5.0% at room temperature and from ∼1.1 to ∼0.70 Wm(-1) K(-1) at 823 K. For the Sn(0.97)Bi(0.03)Te-3% SrTe sample, this leads to a ZT of 1.2 at 823 K and a high average ZT (for SnTe) of 0.7 in the temperature range of 300-823 K, suggesting that SnTe is a robust candidate for medium-temperature thermoelectric applications.

255 citations


Journal ArticleDOI
TL;DR: Cornelissen et al. as discussed by the authors developed a linear response transport theory of diffusive spin and heat transport by magnons in magnetic insulators with metallic contacts, where magnons are described by a position-dependent temperature and chemical potential that are governed by diffusion equations with characteristic relaxation lengths.
Abstract: We develop a linear-response transport theory of diffusive spin and heat transport by magnons in magnetic insulators with metallic contacts. The magnons are described by a position-dependent temperature and chemical potential that are governed by diffusion equations with characteristic relaxation lengths. Proceeding from a linearized Boltzmann equation, we derive expressions for length scales and transport coefficients. For yttrium iron garnet (YIG) at room temperature we find that long-range transport is dominated by the magnon chemical potential. We compare the model's results with recent experiments on YIG with Pt contacts [L. J. Cornelissen, Nat. Phys. 11, 1022 (2015)1745-247310.1038/nphys3465] and extract a magnon spin conductivity of σm=5×105 S/m. Our results for the spin Seebeck coefficient in YIG agree with published experiments. We conclude that the magnon chemical potential is an essential ingredient for energy and spin transport in magnetic insulators.

253 citations


Journal ArticleDOI
TL;DR: In this paper, a paintable/printable thermoelectric material, comprised exclusively of organic components, polyaniline (PANi), graphene, and double-walled nanotube (DWNT) are alternately deposited from aqueous solutions using the layer-by-layer assembly technique.
Abstract: In an effort to create a paintable/printable thermoelectric material, comprised exclusively of organic components, polyaniline (PANi), graphene, and double-walled nanotube (DWNT) are alternately deposited from aqueous solutions using the layer-by-layer assembly technique. Graphene and DWNT are stabilized with an intrinsically conductive polymer, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). An 80 quadlayer thin film (≈1 μm thick), comprised of a PANi/graphene-PEDOT:PSS/PANi/DWNT-PEDOT:PSS repeating sequence, exhibits unprecedented electrical conductivity (σ ≈ 1.9 × 105 S m−1) and Seebeck coefficient (S ≈ 120 μV K−1) for a completely organic material. These two values yield a thermoelectric power factor (PF = S 2 σ −1) of 2710 μW m−1 K−2, which is the highest value ever reported for a completely organic material and among the highest for any material measured at room temperature. These outstanding properties are attributed to the highly ordered structure in the multilayer assembly. This water-based thermoelectric nanocomposite is competitive with the best inorganic semiconductors (e.g., bismuth telluride) at room temperature and can be applied as a coating to any flexible surface (e.g., fibers in clothing). For the first time, there is a real opportunity to harness waste heat from unconventional sources, such as body heat, to power devices in an environmentally-friendly way.

Journal ArticleDOI
TL;DR: In this paper, the authors present an overview on the various aspects of device development i.e. from synthesis of high ZT thermoelectric materials to issues & design aspects of the TEG.

Journal ArticleDOI
TL;DR: A significantly large thermoelectric power factor of ∼31.4 μW/cm·K2 at 856 K in Ag and In co-doped SnTe is reported, which is the highest power factor so far reported for SnTe-based material, which arises from the synergistic effects ofAg and In on the electronic structure and the improved electrical transport properties of SnTe.
Abstract: Understanding the basis of electronic transport and developing ideas to improve thermoelectric power factor are essential for production of efficient thermoelectric materials. Here, we report a significantly large thermoelectric power factor of ∼31.4 μW/cm·K2 at 856 K in Ag and In co-doped SnTe (i.e., SnAgxInxTe1+2x). This is the highest power factor so far reported for SnTe-based material, which arises from the synergistic effects of Ag and In on the electronic structure and the improved electrical transport properties of SnTe. In and Ag play different but complementary roles in modifying the valence band structure of SnTe. In-doping introduces resonance levels inside the valence bands, leading to a significant improvement in the Seebeck coefficient at room temperature. On the other hand, Ag-doping reduces the energy separation between light- and heavy-hole valence bands by widening the principal band gap, which also results in an improved Seebeck coefficient. Additionally, Ag-doping in SnTe enhances the...

Journal ArticleDOI
TL;DR: Flexible thin films of poly(nickel-ethylenetetrathiolate) prepared by an electrochemical method display promising n-type thermoelectric properties with the highest ZT value up to 0.3 at room temperature.
Abstract: Flexible thin films of poly(nickel-ethylenetetrathiolate) prepared by an electrochemical method display promising n-type thermoelectric properties with the highest ZT value up to 0.3 at room temperature. Coexistence of high electrical conductivity and high Seebeck coefficient in this coordination polymer is attributed to its degenerate narrow-bandgap semiconductor behavior.

Journal ArticleDOI
TL;DR: In this article, the authors present an overview and preliminary analysis of computed thermoelectric properties for more than 48,000 inorganic compounds from the Materials Project (MP) and compare their calculations with available experimental data to evaluate the accuracy of different approximations in predicting thermogenesis properties.
Abstract: We present an overview and preliminary analysis of computed thermoelectric properties for more than 48 000 inorganic compounds from the Materials Project (MP). We compare our calculations with available experimental data to evaluate the accuracy of different approximations in predicting thermoelectric properties. We observe fair agreement between experiment and computation for the maximum Seebeck coefficient determined with MP band structures and the BoltzTraP code under a constant relaxation time approximation (R2 = 0.79). We additionally find that scissoring the band gap to the experimental value improves the agreement. We find that power factors calculated with a constant and universal relaxation time approximation show much poorer agreement with experiment (R2 = 0.33). We test two minimum thermal conductivity models (Clarke and Cahill–Pohl), finding that both these models reproduce measured values fairly accurately (R2 = 0.82) using parameters obtained from computation. Additionally, we analyze this data set to gain broad insights into the effects of chemistry, crystal structure, and electronic structure on thermoelectric properties. For example, our computations indicate that oxide band structures tend to produce lower power factors than those of sulfides, selenides, and tellurides, even under the same doping and relaxation time constraints. We also list families of compounds identified to possess high valley degeneracies. Finally, we present a clustering analysis of our results. We expect that these studies should help guide and assess future high-throughput computational screening studies of thermoelectric materials.

Journal ArticleDOI
TL;DR: In this paper, the authors reported the greatly enhanced thermoelectric performance of a ZrS2 monolayer by the biaxial tensile strain, due to the simultaneous increase of the Seebeck coefficient and decrease of the thermal conductivity.
Abstract: The increase of a thermoelectric material's figure of merit (ZT value) is limited by the interplay of the transport coefficients. Here we report the greatly enhanced thermoelectric performance of a ZrS2 monolayer by the biaxial tensile strain, due to the simultaneous increase of the Seebeck coefficient and decrease of the thermal conductivity. Based on first-principles calculations combined with the Boltzmann transport theory, we predict that the band structure of the ZrS2 monolayer can be effectively engineered by the strain, and the Seebeck coefficient is significantly increased. The thermal conductivity is reduced by the applied tensile strain due to the phonon softening. At the strain of 6%, the maximum ZT value of 2.4 is obtained for the p-type doped ZrS2 monolayer at 300 K, which is 4.3 times larger than that of the unstrained system. Moreover, the temperature dependence of the ZT values is investigated, and compared with the unstrained system, the ZT values of the p- and n-type doping are much more balanced by the applied strain.

Journal ArticleDOI
TL;DR: A theory of the thermoelectric conversion efficiency of the SSE device is presented, which clarifies the difference between the S SE and conventional thermoelectedric effects and the efficiency limit of theSSE device.
Abstract: The spin Seebeck effect (SSE) refers to the generation of a spin current as a result of a temperature gradient in magnetic materials including insulators. The SSE is applicable to thermoelectric generation because the thermally generated spin current can be converted into a charge current via spin-orbit interaction in conductive materials adjacent to the magnets. The insulator-based SSE device exhibits unconventional characteristics potentially useful for thermoelectric applications, such as simple structure, device-design flexibility, and convenient scaling capability. In this article, we review recent studies on the SSE from the viewpoint of thermoelectric applications. Firstly, we introduce the thermoelectric generation process and measurement configuration of the SSE, followed by showing fundamental characteristics of the SSE device. Secondly, a theory of the thermoelectric conversion efficiency of the SSE device is presented, which clarifies the difference between the SSE and conventional thermoelectric effects and the efficiency limit of the SSE device. Finally, we show preliminary demonstrations of the SSE in various device structures for future thermoelectric applications and discuss prospects of the SSE-based thermoelectric technologies.

Journal ArticleDOI
TL;DR: This approach leads to a thermoelectric figure of merit increase to 0.13 at 300 K, a factor ∼1,000 times greater than previously reported bulk single-crystal SnS2.
Abstract: In general, in thermoelectric materials the electrical conductivity σ and thermal conductivity κ are related and thus cannot be controlled independently. Previously, to maximize the thermoelectric figure of merit in state-of-the-art materials, differences in relative scaling between σ and κ as dimensions are reduced to approach the nanoscale were utilized. Here we present an approach to thermoelectric materials using tin disulfide, SnS2, nanosheets that demonstrated a negative correlation between σ and κ. In other words, as the thickness of SnS2 decreased, σ increased whereas κ decreased. This approach leads to a thermoelectric figure of merit increase to 0.13 at 300 K, a factor ∼1,000 times greater than previously reported bulk single-crystal SnS2. The Seebeck coefficient obtained for our two-dimensional SnS2 nanosheets was 34.7 mV K(-1) for 16-nm-thick samples at 300 K.

Journal ArticleDOI
TL;DR: In this paper, the biaxial strain dependence of electronic structures and thermoelectric properties (both electron and phonon parts) of monolayer PtSe2 with generalized gradient approximation (GGA) plus spin-orbit coupling (SOC) for the electron part and GGA for the phonon part.
Abstract: Strain engineering is a very effective method to tune the electronic, optical, topological and thermoelectric properties of materials. In this work, we systematically study the biaxial strain dependence of electronic structures and thermoelectric properties (both electron and phonon parts) of monolayer PtSe2 with generalized gradient approximation (GGA) plus spin–orbit coupling (SOC) for the electron part and GGA for the phonon part. The calculated results show that compressive or tensile strain can induce a change in the position of the conduction band minimum (CBM) or valence band maximum (VBM), which produces important effects on the Seebeck coefficient. It is found that compressive or tensile strain can induce significantly enhanced n- or p-type Seebeck coefficients at the critical strain of change for the position of the CBM or VBM, which can be explained by strain-induced band convergence. Based on GGA+U+SOC, the electron correlation effects on the electron transport coefficients are also considered, the corresponding results agree well with those using GGA+SOC. Another essential strain effect is that tensile strain can produce significantly reduced lattice thermal conductivity, and the room temperature lattice thermal conductivity at the strain of −4.02% can decrease by about 60% compared to the unstrained one, which is very favorable for high ZT. To estimate the efficiency of thermoelectric conversion, the figure of merit ZT can be obtained by the empirical scattering time τ. The calculated ZT values show that strain is indeed a very effective strategy to achieve enhanced thermoelectric properties, especially for p-type doping. Tuning thermoelectric properties with strain can also be applied to other semiconducting transition-metal dichalcogenide monolayers MX2 (M = Zr, Hf, Mo, W and Pt; X = S, Se and Te).

Journal ArticleDOI
TL;DR: At high temperature the TEP is substantially larger than the prediction of the Mott relation, approaching to the hydrodynamic limit due to strong inelastic scattering among the charge carriers, however, closer to room temperature the inELastic carrier-optical-phonon scattering becomes more significant and limits theTEP below thehydrodynamic prediction.
Abstract: We report the enhancement of the thermoelectric power (TEP) in graphene with extremely low disorder. At high temperature we observe that the TEP is substantially larger than the prediction of the Mott relation, approaching to the hydrodynamic limit due to strong inelastic scattering among the charge carriers. However, closer to room temperature the inelastic carrier-optical-phonon scattering becomes more significant and limits the TEP below the hydrodynamic prediction. We support our observation by employing a Boltzmann theory incorporating disorder, electron interactions, and optical phonons.

Journal ArticleDOI
TL;DR: In this article, the binodal and spinodal curves in the isopleths of n-type TiNiSn and ZrNiSn were calculated in order to optimize heat treatment conditions.

Journal ArticleDOI
TL;DR: In this paper, the authors suggest a simple way to address this issue through the addition of a small amount of liquid phase exfoliated MoS2 nanosheets into poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) solutions by direct vacuum filtration.
Abstract: For organic thermoelectric materials, a main challenge is to achieve high electrical conductivity and a large Seebeck coefficient, in order to improve the power factor. Here we suggest a simple way to address this issue through the addition of a small amount of liquid-phase exfoliated MoS2 nanosheets into poly(3,4-ethylenedioxythiophene):poly(4-styrenesulfonate) (PEDOT:PSS) solutions by direct vacuum filtration. The effects of exfoliated MoS2 nanosheets in common organic solvents on the thermoelectric properties of PEDOT:PSS were investigated. The organic solvent-assisted exfoliated MoS2 nanosheet solution was found to play an important role in improving the thermoelectric performance of the PEDOT:PSS thin film. Common organic solvents effectively removed some of the PSS during the formation of the film, resulting in a significantly enhanced electrical conductivity (1250 S cm−1) for the PEDOT:PSS/MoS2 (PM) thin film. On the other hand, the introduction of MoS2 nanosheets in PEDOT:PSS led to a slight increase of the Seebeck coefficient from 14.5 to 19.5 μV K−1 without a significant reduction of the electrical conductivity of the PM thin film. An optimized power factor of 45.6 μW m−1 K−2 was achieved for the PM thin film with 4 wt% MoS2 exfoliated in an N,N-dimethylformamide (DMF) solution. The exfoliated MoS2 nanosheets in DMF exhibited a better effect on the thermoelectric performance of the PM composites than did those in other organic solvents. The method used here suggests a novel strategy for improving both electrical conductivity and the Seebeck coefficient, and hence optimizing the thermoelectric performance of the PEDOT:PSS thin film.

Journal ArticleDOI
TL;DR: In this article, a structural transition from a rhombohedral phase to an orthorhombic phase was demonstrated for Te-free Bi2−xSbxSe3.
Abstract: Semiconductors with converging multiple electronic valleys and soft chemical bonds are ideal for high-performance thermoelectrics. Narrow gap Bi2Se3 is a well-known three-dimensional topological insulator with non-trivial surface states, while possessing low thermoelectric properties due to its single-degenerate band conduction, despite being an important constituent of highly efficient n-type thermoelectric Bi2(Te,Se)3. Here we demonstrate that in Te-free Bi2−xSbxSe3 converging multiple electronic band valleys and strengthening phonon scattering can be realized simultaneously via a composition-induced (Sb-alloying) structural transition from a rhombohedral phase to an orthorhombic phase. The accompanying chemical bond softening and structural distortion cause significant modifications to the electronic band structure and phonon dispersion. The convergence of heavy bands realized in the orthorhombic phase (x ≥ 1.0) largely increases the electron density of states effective mass, and thus gives rise to a high Seebeck coefficient of ∼−280 μV K−1 at 800 K. Meanwhile, phonon softening and substantial lattice anharmonicity pertain to weak interchain interactions considerably block the heat-carrying acoustic phonons, resulting in ultralow lattice thermal conductivities of ∼0.6 W m−1 K−1 at 300 K and ∼0.3 W m−1 K−1 at 800 K. Consequently, a maximum thermoelectric figure of merit ZT of ∼1.0 can be achieved for n-type BiSbSe3, about three times higher than that of the optimized Bi2Se3. The moderately high ZT of Te-free BiSbSe3 makes it a promising candidate for low-mid temperature power generations. Furthermore, the concept of structural transition driven band convergence and chemical bond softening can be applied to improve the thermoelectric properties of other materials and may also shed light on identifying new materials.

Journal ArticleDOI
TL;DR: A new p-type thermoelectric material, CsAg5 Te3, is presented that exhibits ultralow lattice thermal conductivity and is attributed to a previously unrecognized phonon scattering mechanism that involves the concerted rattling of a group of Ag ions that strongly raises the Grüneisen parameters of the material.
Abstract: Thermoelectric (TE) materials convert heat energy directly into electricity, and introducing new materials with high conversion efficiency is a great challenge because of the rare combination of interdependent electrical and thermal transport properties required to be present in a single material. The TE efficiency is defined by the figure of merit ZT=(S2σ) T/κ, where S is the Seebeck coefficient, σ is the electrical conductivity, κ is the total thermal conductivity, and T is the absolute temperature. A new p-type thermoelectric material, CsAg5Te3, is presented that exhibits ultralow lattice thermal conductivity (ca. 0.18 Wm−1 K−1) and a high figure of merit of about 1.5 at 727 K. The lattice thermal conductivity is the lowest among state-of-the-art thermoelectrics; it is attributed to a previously unrecognized phonon scattering mechanism that involves the concerted rattling of a group of Ag ions that strongly raises the Gruneisen parameters of the material.

Journal ArticleDOI
TL;DR: The experiments show that the spin Nernst and the spin Hall effect in Pt are of comparable magnitude, but differ in sign, as corroborated by first-principles calculations.
Abstract: The observation of the spin Hall effect triggered intense research on pure spin current transport. With the spin Hall effect, the spin Seebeck effect, and the spin Peltier effect already observed, our picture of pure spin current transport is almost complete. The only missing piece is the spin Nernst (-Ettingshausen) effect, that so far has only been discussed on theoretical grounds. Here, we report the observation of the spin Nernst effect. By applying a longitudinal temperature gradient, we generate a pure transverse spin current in a Pt thin film. For readout, we exploit the magnetization-orientation-dependent spin transfer to an adjacent Yttrium Iron Garnet layer, converting the spin Nernst current in Pt into a controlled change of the longitudinal thermopower voltage. Our experiments show that the spin Nernst and the spin Hall effect in Pt are of comparable magnitude, but differ in sign, as corroborated by first-principles calculations.

Journal ArticleDOI
TL;DR: An electric field tuning of the thermopower in ultrathin WSe2 single crystals over a wide range of carrier concentration by using electric double-layer (EDL) technique is reported.
Abstract: We report an electric field tuning of the thermopower in ultrathin WSe2 single crystals over a wide range of carrier concentration by using electric double-layer (EDL) technique. We succeeded in the optimization of power factor not only in the hole but also in the electron side, which has never been chemically accessed. The maximized values of power factor are one-order larger than that obtained by changing chemical composition, reflecting the clean nature of electrostatic doping.

Journal ArticleDOI
TL;DR: It is shown that the thermoelectric performance of graphene can be significantly improved by using hexagonal boron nitride (hBN) substrates instead of SiO2, and that the Seebeck coefficient provides a direct measure of substrate-induced random potential fluctuations.
Abstract: Fast and controllable cooling at nanoscales requires a combination of highly efficient passive cooling and active cooling. Although passive cooling in graphene-based devices is quite effective due to graphene's extraordinary heat conduction, active cooling has not been considered feasible due to graphene's low thermoelectric power factor. Here, we show that the thermoelectric performance of graphene can be significantly improved by using hexagonal boron nitride (hBN) substrates instead of SiO2 We find the room temperature efficiency of active cooling in the device, as gauged by the power factor times temperature, reaches values as high as 10.35 W⋅m-1⋅K-1, corresponding to more than doubling the highest reported room temperature bulk power factors, 5 W⋅m-1⋅K-1, in YbAl3, and quadrupling the best 2D power factor, 2.5 W⋅m-1⋅K-1, in MoS2 We further show that the Seebeck coefficient provides a direct measure of substrate-induced random potential fluctuations and that their significant reduction for hBN substrates enables fast gate-controlled switching of the Seebeck coefficient polarity for applications in integrated active cooling devices.

Journal ArticleDOI
TL;DR: In this paper, two doping methods were compared: vapor deposition of (tridecafluoro-1,1,2,2-tetrahydrooctyl)trichlorosilane (FTS) or immersion in a solvent containing 4-ethylbenzenesulfonic acid (EBSA).
Abstract: We demonstrate how processing methods affect the thermoelectric properties of thin films of a high mobility semiconducting polymer, PBTTT. Two doping methods were compared: vapor deposition of (tridecafluoro-1,1,2,2-tetrahydrooctyl)trichlorosilane (FTS) or immersion in a solvent containing 4-ethylbenzenesulfonic acid (EBSA). Thermally annealed, thin films doped by FTS deposited from vapor yield a high Seebeck coefficient (α) at high electronic conductivity (σ) and, in turn, a large power factor (PF = α2σ) of ∼100 μW m–1 K–2. The FTS-doped films yield α values that are a factor of 2 higher than the EBSA-doped films at comparable high value of σ. A detailed analysis of X-ray scattering experiments indicates that perturbations in the local structure from either dopant are not significant enough to account for the difference in α. Therefore, we postulate that an increase in α arises from the entropic vibrational component of α or changes in scattering of carriers in disordered regions in the film.

Journal ArticleDOI
TL;DR: In this paper, a promising thermoelectric figure of merit, zT of ∼1.3 at 725 K was obtained in high quality crystalline ingots of Ge1−xBixTe.
Abstract: A promising thermoelectric figure of merit, zT, of ∼1.3 at 725 K was obtained in high quality crystalline ingots of Ge1−xBixTe. The substitution of Bi3+ in a Ge2+ sublattice of GeTe significantly reduces the excess hole concentration due to the aliovalent donor dopant nature of Bi3+. Reduction in carrier density optimizes electrical conductivity, and subsequently enhances the Seebeck coefficient in Ge1−xBixTe. More importantly, a low lattice thermal conductivity of ∼1.1 W m−1 K−1 for Ge0.90Bi0.10Te was achieved, which is due to the collective phonon scattering from meso-structured grain boundaries, nano-structured precipitates, nano-scale defect layers, and solid solution point defects. We have obtained a reasonably high mechanical stability for the Ge1−xBixTe samples. The measured Vickers microhardness value of the high performance sample is ∼165 HV, which is comparatively higher than that of state-of-the-art thermoelectric materials, such as PbTe, Bi2Te3, and Cu2Se.

Journal ArticleDOI
TL;DR: The experimental observation of spin-dependent thermoelectric currents in superconductor-ferromagnet tunnel junctions in high magnetic fields proves the coupling of spin and heat transport in high-field superconductors.
Abstract: We report on the experimental observation of spin-dependent thermoelectric currents in superconductor-ferromagnet tunnel junctions in high magnetic fields. The thermoelectric signals are due to a spin-dependent lifting of the particle-hole symmetry, and are found to be in excellent agreement with recent theoretical predictions. The maximum Seebeck coefficient inferred from the data is about -100 μV/K, much larger than commonly found in metallic structures. Our results directly prove the coupling of spin and heat transport in high-field superconductors.