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At least 253 records · Page 14

A chemical kinetics perspective on thermoelectric transport

There is a growing community of chemists and materials scientists exploring thermoelectric properties of organic, polymeric, hybrid, and composite materials. Many of these materials are nondegenerate semiconductors, meaning that the Fermi and transport charge transport energy levels are significantly offset. Others are ionic conductors. While the meaning of the essential parameters electrical conductivity (σ) and Seebeck coefficient (S, the voltage difference per degree of temperature difference) are accessible, the origins of S are not readily apparent to one trained mainly in chemistry. The purpose of this manuscript is to illustrate S as being the result of a steady state difference between concentrations of two designations of charge carriers, those on hotter and those on colder sides of a material sample, analogous to the equilibrium among interconverting chemical species that differ in enthalpy and entropy. The ion-based Seebeck coefficient, also known as the Soret effect, can be explained using principles similar to those applicable to electrons and holes. We hope that this analysis leads to wider understanding of the origins of S through an explanation using the language of chemical kinetics and thermodynamics, and appreciation of ways that thermoelectric efficiency can be enhanced in emerging materials.

36 MATERIALS SCIENCE↗

Challenges of measuring spin Seebeck noise

Just as electronic shot noise in driven conductors results from the granularity of charge and the statistical variation in the arrival times of charge carriers, there are predictions for fundamental noise in magnon currents due to angular momentum being carried by discrete excitations. The inverse spin Hall effect as a transduction mechanism to convert spin current into charge current raises the prospect of experimental investigations of such magnon shot noise. Spin Seebeck effect measurements have demonstrated the electrical detection of thermally driven magnon currents and have been suggested as an avenue for accessing spin current fluctuations. Using spin Seebeck structures made from yttrium iron garnet on gadolinium gallium garnet, we demonstrate the technical challenges inherent in such noise measurements. While there is a small increase in voltage noise in the inverse spin Hall detector at low temperatures associated with adding a magnetic field, the dependence on field orientation implies that this is not due to magnon shot noise. We describe theoretical predictions for the expected magnitude of magnon shot noise, highlighting ambiguities that exist. Further, we show that magnon shot noise detection through the standard inverse spin Hall approach is likely impossible due to geometric factors. Implications for future attempts to measure magnon shot noise are discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photo-controllable thermoelectric properties with reversibility and photo-thermoelectric effects of tungsten trioxide accompanied by its photochromic phenomenon

The addition of photo-controllable properties to tungsten trioxide (WO{sub 3}) is of interest for developing practical applications of WO{sub 3} as well as for interpreting such phenomena from scientific viewpoints. Here, a sputtered crystalline WO{sub 3} thin film generated thermoelectric power due to ultraviolet (UV) light-induced band-gap excitation and was accompanied by a photochromic reaction resulting from generating W{sup 5+} ions. The thermoelectric properties (electrical conductivity (σ) and Seebeck coefficient (S)) and coloration of WO{sub 3} could be reversibly switched by alternating the external stimulus between UV light irradiation and dark storage. After irradiating the film with UV light, σ increased, whereas the absolute value of S decreased, and the photochromic (coloration) reaction was detected. Notably, the opposite behavior was exhibited by WO{sub 3} after dark storage, and this reversible cycle could be repeated at least three times. Moreover, photo-thermoelectric effects (photo-conductive effect (photo-conductivity, σ{sub photo}) and photo-Seebeck effect (photo-Seebeck coefficient, S{sub photo})) were also detected in response to visible-light irradiation of the colored WO{sub 3} thin films. Under visible-light irradiation, σ{sub photo} and the absolute value of S{sub photo} increased and decreased, respectively. These effects are likely attributable to the excitation of electrons from the mid-gap visible light absorption band (W{sup 5+} state) to the conduction band of WO{sub 3}. Our findings demonstrate that the simultaneous, reversible switching of multiple properties of WO{sub 3} thin film is achieved by the application of an external stimulus and that this material exhibits photo-thermoelectric effects when irradiated with visible-light.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photo- and gas-tuned, reversible thermoelectric properties and anomalous photo-thermoelectric effects of platinum-loaded tungsten trioxide

We report the photo- and gas-controllable properties of platinum-loaded tungsten trioxide (Pt/WO{sub 3}), which is of interest for developing practical applications of WO{sub 3} as well as for interpreting such phenomena from scientific viewpoints. Here, a Pt/WO{sub 3} thin film generated a thermoelectric power due to the ultraviolet-light-induced band-gap excitation (photochromic (PC) reaction) and/or dark storage in formic acid vapor (gaschromic (GC) reaction) in the absence of O{sub 2}, resulting from the generation of W{sup 5+} ions. After such chromic reactions, the electrical conductivity (σ) is increased, whereas the absolute value of the Seebeck coefficient (S) is decreased. The changes in σ and S and their rate of change for consistency increased in the order of: during the PC reaction < during the GC reaction < during simultaneous PC and GC reactions. The opposite behaviors, a decrease in σ and an increase in S, were exhibited by Pt/WO{sub 3} in the presence of O{sub 2} after dark storage or visible-light irradiation. This reversible cycle could be repeated. Moreover, anomalous, nontrivial photo-thermoelectric effects (a photoconductive effect (photoconductivity, σ{sub photo}) and a photo-Seebeck effect (photo-Seebeck coefficient, S{sub photo})) were also detected in response to the visible-light irradiation of Pt/WO{sub 3} in the absence of O{sub 2} after chromic reactions. Under visible-light irradiation, both σ{sub photo} and the absolute value of S{sub photo} are increased. After the irradiation, both values were decreased, that is, σ and the absolute value of S were smaller than σ{sub photo} and the absolute value of S{sub photo}, respectively. These effects are likely to be due to the photoinduced charge carriers and the accumulated electrons in Pt contributing to the increase in σ{sub photo}. In addition, electrons are extracted from the W{sup 5+} state, decreasing the number of W{sup 5+} in H{sub x}WO{sub 3} and thus contributing to the increase in S{sub photo}. After light irradiation, the accumulated electrons in Pt are returned to the energetically favorable W{sup 5+} state, and Pt/H{sub x}WO{sub 3} are returned to the initial state. Then both σ and S are decreased. The mechanisms of our anomalous, nontrivial photo-thermoelectric effects are presumed to be different from that involving the two-carrier contribution to the transport properties.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Ni and Se co-doping increases the power factor and thermoelectric performance of CoSbS

In this paper, we present a new investigation on paracostibite (CoSbS), a potential thermoelectric material for power generation in the intermediate temperature range (700–900 K) consisting of earth abundant elements. We report an improved synthesis of single phase materials of Co 1–x Ni x SbS 1–y Se y (x = 0–0.07, y = 0–0.09) using vacuum melting and annealing followed by SPS processing. The effects of Ni and Se co-doping on the electronic and thermal transport properties of CoSbS were investigated. Doping with Ni on the Co site increases the carrier concentration and moves the Fermi level deep into the conduction band, producing an enhanced power factor. First-principles electronic band structure calculations indicate a multi valley nature of the conduction band where Ni doping leads to n-type behaviour and a sharp increase of the density of states effective mass, enhancing the Seebeck coefficient. Unlike the Ni doping which has little effect on thermal transport, alloying Se on the S site intensifies the alloying scattering resulting in a lower lattice thermal conductivity of 2.4 W m –1 K –1 at 900 K for Co 0.93 Ni 0.07 SbS 0.93 Se 0.07 . Alloying Se on the S site of the structure further boosts the power factor to 22 μW cm –1 K –2 and leads to a maximum ZT of 0.58 at 900 K, which is the best ZT value achieved in the system.

36 MATERIALS SCIENCE↗

Transverse thermal energy conversion using spin and topological structures

Conversion of thermal to electrical energy has been a subject of intense study for well over two centuries. Despite steady progress throughout the past several decades, solid-state thermoelectric (TE) energy conversion devices remain adequate only for niche applications. One appealing option for circumventing the limits of conventional TE physics is to utilize phenomena where flows of heat and charge are perpendicular, the so-called “transverse” geometry. In this Tutorial, we discuss recent advances behind new ways to generate large transverse thermoelectric voltages, such as the spin Seebeck and Nernst effects, as well as Weyl physics. We provide suggestions for how these mechanisms might be enhanced and implemented into high-efficiency, next generation transverse TE devices. Furthermore, we also discuss best practices for accurate measurement and reporting of transverse thermoelectric material properties, including a case study of a round robin spin Seebeck coefficient measurement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Characterization Report on Fuels for NEAMS Model Validation

ABSTRACT U3Si2 has become a material of interest for its potential as an accident tolerant fuel used in commercial light water reactors. In order to better understand the nature of the 5f-electrons and mechanisms that govern electrical and heat transport in U3Si2, and to accurately model this compound at all relevant temperatures we have performed detailed studies of this material by means of the heat capacity, electrical resistivity, Seebeck and Hall effects, and thermal conductivity. Polycrystalline samples of U3Si2 were prepared by arc-melting stoichiometric amounts of elemental U and Si. All the results obtained, especially small magneto-resistivity, large low-temperature heat capacity, and characteristic dependence of the Seebeck coefficient, point to delocalized nature of 5f-electrons in U3Si2. The thermal conductivity is ~8.5 W/m-K at room temperature and we show that the lattice part of the total thermal conductivity is small, with electrons dominating heat transport above 300 K. This knowledge of the details of the heat transport in U3Si2 will be useful for researchers working on modeling and simulations of this new advanced fuel.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Synthesis, electronic transport and optical properties of Si:α-Fe 2 O 3 single crystals

We report the synthesis of silicon-doped hematite (Si:α-Fe2O3) single crystals via chemical vapor transport, with Si incorporation on the order of 1019 cm-3. The conductivity, Seebeck and Hall effect were measured in the basal plane between 200 and 400 K. Distinct differences in electron transport were observed above and below the magnetic transition temperature of hematite at ~265 K (the Morin transition, TM). Above 265 K, transport was found to agree with the adia-batic small-polaron model, the conductivity was characterized by an activation energy of ~100 meV and the Hall effect was dominated by the weak ferromagnetism of the material. A room temperature electron drift mobility of ~10-2 cm2 V-1 s-1 was estimated. Below TM, the activation energy increased to ~160 meV and a conventional Hall coefficient could be de-termined. In this regime, the Hall coefficient was negative and the corresponding Hall mobility was temperature-independent with a value of ~10-1 cm2 V-1 s-1. Seebeck coefficient measurements indicated that the silicon donors were fully ionized in the temperature range studied. Finally, in the doped species we observe a very broad infrared absorption fea-ture centered near 0.4 eV that does not appear to be hydroxyl related but is tentatively assigned to photon-assisted small-polaron hops. These results are discussed in the context of existing hematite transport studies.

Rettie, Alexander J. E.↗

Thermal and transport properties of U 3 Si 2

Here, we have studied U 3 Si 2 by means of the heat capacity, electrical resistivity, Seebeck and Hall effects, and thermal conductivity in the temperature range 2-300 K and in magnetic fields up to 9 T. All the results obtained point to delocalized nature of 5f-electrons in this material. The low temperature heat capacity is enhanced (γ el ~ 150 mJ/mol-K 2 ) and shows an upturn in C p / T (T), characteristic of spin fluctuations. The thermal conductivity of U 3 Si 2 is ~8.5 W/m-K at room temperature and we show that the lattice part of the total thermal conductivity is small, with electrons dominating heat transport above 300 K.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

An ab initio electronic transport database for inorganic materials

Electronic transport in materials is governed by a series of tensorial properties such as conductivity, Seebeck coefficient, and effective mass. These quantities are paramount to the understanding of materials in many fields from thermoelectrics to electronics and photovoltaics. Transport properties can be calculated from a material’s band structure using the Boltzmann transport theory framework. We present here the largest computational database of electronic transport properties based on a large set of 48,000 materials originating from the Materials Project database. Our results were obtained through the interpolation approach developed in the BoltzTraP software, assuming a constant relaxation time. We present the workflow to generate the data, the data validation procedure, and the database structure. In conclusion, our aim is to target the large community of scientists developing materials selection strategies and performing studies involving transport properties.

36 MATERIALS SCIENCE↗

Origins of large light induced voltage in magnetic tunnel junctions grown on semiconductor substrates

Recently, the study of interactions between electron spins and heat currents has given rise to the field of “Spin Caloritronics”. Experimental studies of these interactions have shown a possibility to combine the use of heat and light to power magnetic tunnel junction (MTJ) devices. Here we present a careful study of an MTJ device on Si substrate that can be powered entirely by light. We analyze the influence of the material properties, device geometry, and laser characteristics on the electric response of the sample. We demonstrate that by engineering the MTJ and its electrical contact, a large photovoltage reaching 100 mV can be generated. This voltage originates from the Si substrate and depends on the MTJ magnetic configuration. Finally, we discuss the origin of the photo-voltage in terms of Seebeck and photovoltaic effects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

RIKEN TRIP Magnets Database

This dataset contains ab-initio calculation results for the temperature-dependent anomalous Hall conductivity, the anomalous Nernst effect, and the Seebeck coefficient. All calculations are based on ab-inito Quantum Espresso (PWSCF v.6.3) + Wannier90 (v.3.0.0). The dependence on carrier doping is also calculated. For all calculations a ferromagnetic order has been assumed, which might not correspond to the true ground state of the system. Tabulated values for the magnetic moments and essential input files for Quantum Espresso are available for download as attachments. This project has been supported by the RIKEN Transformative Research Innovation Platform (TRIP), Use Case: Many-body Electron Systems.

36 MATERIALS SCIENCE↗

Thermomagnetic phenomena in the mixed state of high temperature superconductors

Galvano- and thermomagnetic-phenomena in high temperature superconductors, based on kinetic coefficients, are discussed, along with a connection between the electric field and the heat flow in superconductor mixed state. The relationship that determines the transport coefficients of high temperature superconductors in the mixed state based on Seebeck and Nernst effects is developed. It is shown that this relationship is true for a whole transition region of the resistive mixed state of a superconductor. Peltier, Ettingshausen and Righi-Leduc effects associated with heat conductivity as related to high temperature superconductors are also addressed.

Meilikhov, E. Z.↗

Synthesis and Optimization of Thermoelectric Properties of Zn(x)Sb3

High-performance thermoelectric materials are studied to investigate their abilities to optimize electrical and minimize thermal conductivities. A stoichiometric range of p-type zinc antimonide compounds was synthesized to analyze the trends in their thermoelectric properties. Zn(x)Sb3 (x=3.80, 3.85, 3.90, 3.95, 4.00, 4.05, 4.10) was reacted at 750 C and annealed at 300 C for 24 hours at each temperature. Electronic transport properties such as Seebeck and Hall Effect were measured to analyze possible trends in the set of compositions. SEM, EDS, and XRD were used to quantify both ingots and hot-pressed samples to confirm that they were single-phase and of the expected stoichiometries. Recent SEM data indicated that Zn(3.90)Sb3 and Zn(4.00)Sb3 samples were actually Zn3Sb2. In hopes of further improving the figure-of-merit (ZT) of the binary system, V, Cr, Mn, Fe, Co, In, and Sn were used to dope (Zn(0.95)M(0.05))(3.95)Sb3.

Doan-Nguyen, Vicky V.↗

Thermoelectric power factor enhancement with gate-all-around silicon nanowires

The thermoelectric properties of gate-all-around silicon nanowires (Si NWs) are calculated to determine the potential for significant power factor enhancement. The Boltzmann transport equation and relaxation time approximation are employed to develop an electron transport model used to determine the field-effect mobility, electrical conductivity, Seebeck coefficient, and power factor for Si NWs with cross-sectional areas between 4 nm × 4 nm and 12 nm × 12 nm and a range of gate biases. Electrical conductivity for the gated Si NWs was much higher than that of doped Si due to the lack of ionized impurities and correspondingly greater carrier mobility. A significant increase in electrical conductivity with decreasing Si NW cross-sectional area was also observed due to a large increase in the average carrier density. For all Si NWs, the Seebeck coefficient was lower than that of doped bulk Si due to the different energy dependence between ionized impurity and phonon-mediated scattering processes. This decrease was also confirmed with Seebeck coefficient measurements of multigated Si NWs and n-type Si thin-films. Quantum confinement was also found to increase the Seebeck coefficient for <8 nm × 8 nm Si NWs and also at high charge densities. A maximum power factor of 6.8 × 10{sup −3} W m{sup −1} K{sup −2} was calculated for the 6 nm × 6 nm Si NWs with typical Si/SiO{sub 2} interface roughness, which is 2–3 × those obtained experimentally for bulk Si. The power factor was also found to greatly depend on surface roughness, with a root-mean-square roughness of <0.8 nm necessary for power factor enhancement. An increase in ZT may also be possible if a low thermal conductivity can be obtained with minimal surface roughness.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Phase-transition-induced thermal hysteresis in Type-II weyl semimetals M o T e 2 and M o 1 − x W x T e 2

The resistivity versus temperature measurement is commonly used for identifying temperature-induced phase-change and the resulting hysteresis loop. However, while the resistance is influenced by both the density of states and the carrier lifetimes, the Seebeck coefficient is influenced predominantly by the density of states, and hence is a better probe of the phase of the material. Here, 1T'-T d temperature-induced phase transition in MoTe 2 is studied using temperature-dependent X-ray diffraction, resistivity, and Seebeck coefficient measurements. A more distinct hysteresis is observed when measuring the Seebeck coefficient which is consistent with direct measurements of the crystallographic angle using the temperature-dependent X-ray diffraction. The Seebeck and electrical resistivity measurements indicate a competing contribution of the electrons and holes. The contribution of electron pockets becomes more dominant when molybdenum atoms are replaced by tungsten. In MoTe 2 , a topologically induced enhancement of the Nernst coefficient is observed at low temperatures and a relatively large phase-transition induced Thomson coefficient of 111 μV∙K -1 is measured at 254 K.

36 MATERIALS SCIENCE↗

Thermomagnetic properties of Bi 2 Te 3 single crystal in the temperature range from 55 K to 380 K

Magnetothermoelectric transport provides an understanding of coupled electron-hole-phonon current in topological materials and has applications in energy conversion and cooling. In this paper, we study the Nernst coefficient, the magneto-Seebeck coefficient, and the magnetoresistance of single-crystalline Bi 2 Te 3 under external magnetic field in the range of –3T to 3T and in the temperature range of 55 K to 380 K. Moreau's relation is employed to justify both the overall trend of the Nernst coefficient and the temperature at which this coefficient changes sign. We observe a nonlinear relationship between the Nernst coefficient and the applied magnetic field in the temperature range of 55 K to 255 K. An increase in both the Nernst coefficient and the magneto-Seebeck coefficient is observed as the temperature is reduced which can be attributed to the increased mobility of the carriers at lower temperatures. First-principles density functional theory calculations were carried out to physically model the experimental data including electronic and transport properties. Simulation findings agreed with the experiments and provide a theoretical insight to justify the measurements.

36 MATERIALS SCIENCE↗

Detailed Uncertainty Analysis of the ZEM-3 Measurement System

The measurement of Seebeck coefficient and electrical resistivity are critical to the investigation of all thermoelectric systems. Therefore, it stands that the measurement uncertainty must be well understood to report ZT values which are accurate and trustworthy. A detailed uncertainty analysis of the ZEM-3 measurement system has been performed. The uncertainty analysis calculates error in the electrical resistivity measurement as a result of sample geometry tolerance, probe geometry tolerance, statistical error, and multi-meter uncertainty. The uncertainty on Seebeck coefficient includes probe wire correction factors, statistical error, multi-meter uncertainty, and most importantly the cold-finger effect. The cold-finger effect plagues all potentiometric (four-probe) Seebeck measurement systems, as heat parasitically transfers through thermocouple probes. The effect leads to an asymmetric over-estimation of the Seebeck coefficient. A thermal finite element analysis allows for quantification of the phenomenon, and provides an estimate on the uncertainty of the Seebeck coefficient. The thermoelectric power factor has been found to have an uncertainty of +9-14 at high temperature and 9 near room temperature.

Seebeck effect↗