Mesoscopic thermal and thermoelectric measurements of individual carbon nanotubes

We discuss the mesoscopic experimental measurements of electron energy dissipation, phonon thermal transport, and thermoelectric phenomena in individual carbon nanotubes. The temperature distributions in electrically heated individual multiwalled carbon nanotubes have been measured with a scanning thermal microscope. The temperature profiles along the tube axis in nanotubes indicate the bulk dissipation of electronic energy to phonons. In addition, thermal conductivity of an individual multiwalled nanotube has been measured using a microfabricated suspended device. The observed thermal conductivity is two orders of magnitude higher than the estimation from previous experiments that used macroscopic mat samples. Finally, we present thermoelectric power (TEP) of individual single walled carbon nanotubes using a novel mesoscopic device. A strong modulation of TEP as a function of the gate electrode was observed.     

Spin-seebeck effect: a phonon driven spin distribution

Here we report on measurements of the spin-Seebeck effect in GaMnAs over an extended temperature range alongside the thermal conductivity, specific heat, magnetization, and thermoelectric power. The amplitude of the spin-Seebeck effect in GaMnAs scales with the thermal conductivity of the GaAs substrate and the phonon-drag contribution to the thermoelectric power of the GaMnAs, demonstrating that phonons drive the spin redistribution. A phenomenological model involving phonon-magnon drag explains the spatial and temperature dependence of the measured spin distribution.     

Positron scattering by phonons in metals

Processes involved in positron-matter interaction are studied. The stopping power and mean free path are calculated for positrons with an energy of about 1 eV, which are scattered mostly by phonons. The mean free path and range of positrons in tungsten, as well as the stopping power of tungsten, are calculated for positron energies between 0.025 and 10 eV.     

A comparison study on the electronic structures,lattice dynamics and thermoelectric properties of bulk silicon and silicon nanotubes

In order to investigate the mechanism of the electron and phonon transport in a silicon nanotube(SiNT),the electronic structures,the lattice dynamics,and the thermoelectric properties of bulk silicon(bulk Si)and a SiNT have been calculated in this work using density functional theory and Boltzmann transport theory.Our results suggest that the thermal conductivity of a SiNT is reduced by a factor of 1,while its electrical conductivity is improved significantly,although the Seebeck coefficient is increased slightly as compared to those of the bulk Si.As a consequence,the figure of merit(ZT)of a SiNT at 1200 K is enhanced by 12 times from 0.08 for bulk Si to 1.10.The large enhancement in electrical conductivity originates from the largely increased density of states at the Fermi energy level and the obviously narrowed band gap.The significant reduction in thermal conductivity is ascribed to the remarkably suppressed phonon thermal conductivity caused by a weakened covalent bonding,a decreased phonon density of states,a reduced phonon vibration frequency,as well as a shortened mean free path of phonons.The other factors influencing the thermoelectric properties have also been studied from the perspective of electronic structures and lattice dynamics.     

Anomalous thermal conductivity of polyacetylene

Measurements of the specific heat and of the thermal conductivity of pure and iodine doped polyacetylene from liquid helium to room temperature are reported. The thermal conductivity rises linearly from 3 to 50 K and with about the third power of the temperature from 50 to 300 K. The kink at 50 K corresponds to a very unusual minimum of the phonon mean free path, probably caused by resonant scattering of fast thermal phonons (which travel along the chains) on low frequency interchain modes. These results suggest that the polymer chains are oriented parallel to the well-known fibers in polyacetylene.     

Reduction of phonon mean free path: From low-temperature physics to room temperature applications in thermoelectricity

It has been proposed for a long time now that the reduction of the thermal conductivity by reducing the phonon mean free path is one of the best way to improve the current performance of thermoelectrics. By measuring the thermal conductance and thermal conductivity of nanowires and thin films, we show different ways of increasing the phonon scattering from low-temperature up to room-temperature experiments. It is shown that playing with the geometry (constriction, periodic structures, nano-inclusions), from the ballistic to the diffusive limit, the phonon thermal transport can be severely altered in single crystalline semiconducting structures; the phonon mean free path is in consequence reduced. The diverse implications on thermoelectric properties will be eventually discussed.     

Minimum thermal conductivity of superlattices

The phonon thermal conductivity of a multilayer is calculated for transport perpendicular to the layers. There is a crossover between particle transport for thick layers to wave transport for thin layers. The calculations show that the conductivity has a minimum value for a layer thickness somewhat smaller then the mean free path of the phonons.     

Theoretical analysis of cross-plane lattice thermal conduction in graphite

A theoretical analysis of the cross-plane lattice thermal conduction in graphite is performed by using first-principles calculations and in the single-mode relaxation time approximation. The out-of-plane phonon acoustic mode ZA and optical mode ZO have almost 80% and 20% of contributions to cross-plane heat transfer, respectively. However, these two branches have a small part of total specific heat above 300 K. Phonons in the central 16% of Brillouin zone contribute80% of cross-plane transport. If the group velocity angle with respect to the graphite layer normal is less than 30?, then the contribution is 50% at 300 K. The ZA phonons with long cross-plane mean free path are focused in the cross-plane direction, and the largest mean free path is on the order of several micrometers at room temperature. The average value of cross-plane mean free path at 300 K is 112 nm for ZA phonons with group velocity angle with respect to the layer normal being less than 15?. The average value is dropped to 15 nm when phonons of all branches in the whole Brillouin zone are taken into account, which happens because most phonons have small or even no contributions.     

Tuning Thermal Conductivity in Si Nanowires with Patterned Structures

Tuning the thermal conductivity of silicon nanowires(Si-NWs)is essential for realization of future thermoelectric devices.The corresponding management of thermal transport is strongly related to the scattering of phonons,which are the primary heat carriers in Si-NWs.Using the molecular dynamics method,we find that the scattering of phonons from internal body defects is stronger than that from surface structures in the low-porosity range.Based on our simulations,we propose the concept of an exponential decay in thermal conductivity with porosity,specifically in the low-porosity range.In contrast,the thermal conductivity of Si-NWs with a higher porosity approaches the amorphous limit,and is insensitive to specific phonon scattering processes.Our findings contribute to a better understanding of the tuning of thermal conductivity in Si-NWs by means of patterned nanostructures,and may provide valuable insights into the optimal design of one-dimensional thermoelectric materials.     

Nanotube phonon waveguide

We find that the high thermal conductivity of carbon nanotubes remains intact under severe structural deformations while the corresponding electrical resistance and thermoelectric power show compromised responses. Similar robust thermal transport against bending is found for boron nitride nanotubes. Surprisingly, for both systems the phonon mean free path exceeds the characteristic length of structural ripples induced by bending and approaches the theoretical limit set by the radius of curvature. The robustness of heat conduction in nanotubes refines the ultimate limit that is far beyond the reach of ordinary materials.     

Thermal transport in heavily deformed and γ -irradiated LiF at temperatures near 1 k

The thermal conductivity κ of heavily deformed LiF crystals has been measured at temperatures T ? 0.5 K following exposure of the samples to γ irradiation. The results are in agreement with recent measurements of ballistic phonon propagation in similar samples at an equivalent temperature of ≈ 4 K. A fraction of the phonons have a mean free path of order 1 cm in the heavily deformed crystal, and γ-irradiation increases the fraction having a long mean free path. The measurements support a dynamic (as opposed to static) model of phonon-dislocation interaction.     

First-principles investigations on elastic,thermodynamic and lattice thermal conductivity of topological insulator LaAs

Topological insulators are always a hot topic owing to their various peculiar physical effects, which are useful in spintronics and quantum information processing. Herein, we systematically investigate the elastic, thermodynamic and lattice thermal conductivity of a new typical topological insulator LaAs by combining the first-principles approach and an iterative solution of the Boltzmann transport equation. The obtained elastic constants and other lattice structural parameters of LaAs are well consistent with the experimental and other theoretical results. For the first time, the lattice thermal conductivity (5.46 W/(m?K)) and mean free path (14.4 nm) of LaAs are obtained,which manifests that the LaAs is more likely to be a desirable thermoelectric material. It is noted that the obtained mode-averaged Grüneisen parameters by different ab initio simulation packages are very similar, suggesting that our results are rather responsible. From the phonon scattering rates of LaAs, we speculate that the reduction of acoustic-optical gap and the larger phonon scattering may jointly result in reduction of thermal conductivity for LaAs. Meanwhile, the temperature dependence curves of the lattice thermal conductivity, heat capacity and phonon mean free path are also presented. We expect our work can provide more information for further experimental studies.     

Interpretation of thermoelectric power behaviour of Zinc nanowire composites: Phonon-scattering mechanism

We develop a theoretical model for quantitative analysis of temperature-dependent thermoelectric power (S) of Zn nanowires. In doing so, we first use the Mott expression to compute the electron diffusive thermoelectric power (S_c^diff.) using Fermi energy as electron-free parameter, S_c^diff. shows linear temperature dependence. Further, the S_c^diff. contribution is subtracted from the experimental data and the difference (S_experimental-S_c^dif) is characterized as phonon drag thermoelectric power (S_ph^drag) which is obtained within the relaxation time approximation where the thermoelectric power is limited by the scattering of phonons with impurities, grain boundaries, charge careers and phonons in the nanowires. The S_ph^drag shows anomalous temperature-dependent behaviour, which is an artifact of various operating scattering mechanisms. The observed anomalies are well accounted in terms of interaction among the phonons-impurity, phonon-grain boundaries, phonon-electron and the umklapp scattering. It is also shown that for phonons the scattering and transport cross-sections are proportional to ω⁴ in the Rayleigh regime where ω is the frequency of the phonons. Numerical analysis of thermoelectric power from the present model shows similar results as those revealed from experiments.     

Thermal conductivity reduction and thermoelectric figure of merit increase by embedding nanoparticles in crystalline semiconductors

Atomic substitution in alloys can efficiently scatter phonons, thereby reducing the thermal conductivity in crystalline solids to the "alloy limit." Using In0.53Ga0.47As containing ErAs nanoparticles, we demonstrate thermal conductivity reduction by almost a factor of 2 below the alloy limit and a corresponding increase in the thermoelectric figure of merit by a factor of 2. A theoretical model suggests that while point defects in alloys efficiently scatter short-wavelength phonons, the ErAs nanoparticles provide an additional scattering mechanism for the mid-to-long-wavelength phonons.     

FeMnAl合金低温声子热导率的反常行为

我们在4.2—30K测量了具有电阻负温度系数的晶态Fe-25Mn-5Al-0.2C合金的热导率,发现其声子热导率主要随温度线性变化,可能是由于Al的加入使电子平均自由程减小,从而对声子散射减弱所致。 关键词：     

Semiconducting large bandgap oxides as potential thermoelectric materials for high-temperature power generation?

Semiconducting large bandgap oxides are considered as interesting candidates for high-temperature thermoelectric power generation (700–1,200 °C) due to their stability, lack of toxicity and low cost, but so far they have not reached sufficient performance for extended application. In this review, we summarize recent progress on thermoelectric oxides, analyze concepts for tuning semiconductor thermoelectric properties with view of their applicability to oxides and determine key drivers and limitations for electrical and thermal transport properties in oxides based on our own experimental work and literature results. For our experimental assessment, we have selected representative multicomponent oxides that range from materials with highly symmetric crystal structure (SrTiO₃ perovskite) over oxides with large densities of planar crystallographic defects (Ti _n O_2n?1 Magnéli phases with a single type of shear plane, NbO _x block structures with intersecting shear planes and WO_3?x with more defective block and channel structures) to layered superstructures (Ca₃Co₄O₉ and double perovskites) and also include a wide range of their composites with a variety of second phases. Crystallographic or microstructural features of these oxides are in 0.3–2 nm size range, so that oxide phonons can efficiently interact with them. We explore in our experiments the effects of doping, grain size, crystallographic defects, superstructures, second phases, texturing and (to a limited extend) processing on electric conductivity, Seebeck coefficient, thermal conductivity and figure of merit. Jonker and lattice-versus-electrical conductivity plots are used to compare specific materials and material families and extract levers for future improvement of oxide thermoelectrics. We show in our work that oxygen vacancy doping (reduction) is a more powerful driver for improving the power factor for SrTiO₃, TiO₂ and NbO _x than heterovalent doping. Based on our Seebeck-conductivity plots, we derived a set of highest achievable power factors. We met these best values in our own experiments for our titanium oxide- and niobium oxide-based materials. For strontium titanate-based materials, the estimated highest power factor was not reached; further material improvement is possible and can be reached for materials with higher carrier densities. Our results show that periodic crystallographic defects and superstructures are most efficient in reducing the lattice thermal conductivity in oxides, followed by hetero- and homovalent doping. Due to the small phonon mean free path in oxides, grain boundary scattering in nanoceramics or materials with nanodispersions is much less efficient. We investigated the impact of texturing in Ca₃Co₄O₉ ceramics on thermoelectric performance; we did not find any improvement in the overall in-plane performance of a textured ceramic compared to the corresponding random ceramic.     

Electron scattering and transport phenomena in small-gap zinc-blende semiconductors

We give expressions for electrical conductivity, thermoelectric power and thermal conductivity of conduction band electrons in small-gap zinc-blende semiconductors, obtained by solving the Boltzmann equation by a variational procedure. The term resulting from the phonon-drag is included in the Boltzmann equation. The following electron scattering mechanisms are investigated: inter and intraband scattering by optical phonons via polar and nonpolar interactions, scattering by charged centers (ionized defects and heavy holes) and by neutral centers, as well as scattering by acoustic phonons. Particular attention is paid to the screening of the electron-optical phonon polar interaction by free carriers, which is particularly important in the case of a linear energy band. The formula for the intraband RPA dielectric function for the case of the linear band is given.The general formulation of all the problems investigated permits direct application of the results given in this paper to both intrinsic or n-type HgTe-type and InSb-type semiconductors, including mixed crystals, e.g. Cd_xHg_1?xSe near the cross point.     

Intrinsically minimal thermal conductivity in cubic I-V-VI2 semiconductors

We report measurements of the thermal conductivity of high-quality crystals of the cubic I-V-VI2 semiconductors AgSbTe2 and AgBiSe2. The thermal conductivity is temperature independent from 80 to 300 K at a value of approximately 0.70 W/mK. Heat conduction is dominated by the lattice term, which we show is limited by umklapp and normal phonon-phonon scattering processes to a value that corresponds to the minimum possible, where the phonon mean free path equals the interatomic distance. Minimum thermal conductivity in cubic I-V-VI2 semiconductors is due to an extreme anharmonicity of the lattice vibrational spectrum that gives rise to a high Grüneisen parameter and strong phonon-phonon interactions. Members of this family of compounds are therefore most promising for thermoelectric applications, particularly as p-type materials.     

Role of disorder and anharmonicity in the thermal conductivity of silicon-germanium alloys: a first-principles study

The thermal conductivity of disordered silicon-germanium alloys is computed from density-functional perturbation theory and with relaxation times that include both harmonic and anharmonic scattering terms. We show that this approach yields an excellent agreement at all compositions with experimental results and provides clear design rules for the engineering of nanostructured thermoelectrics. For Si(x)Ge(1-x), more than 50% of the heat is carried at room temperature by phonons of mean free path greater than 1 μm, and an addition of as little as 12% Ge is sufficient to reduce the thermal conductivity to the minimum value achievable through alloying. Intriguingly, mass disorder is found to increase the anharmonic scattering of phonons through a modification of their vibration eigenmodes, resulting in an increase of 15% in thermal resistivity.