The generalization of the Local Density Approximation (LDA) method for the systems with strong Coulomb correlations is presented which gives a correct description of the Mott insulators. The LDA+U method is based on the model hamiltonian approach and allows to take into account the non-sphericity of the Coulomb and exchange interactions. parameters. Orbital-dependent LDA+U potential gives correct orbital polarization and corresponding Jahn-Teller distortion. To calculate the spectra of the strongly correlated systems the impurity Anderson model should be solved with a many-electron trial wave function. All parameters of the many-electron hamiltonian are taken from LDA+U calculations. The method was applied to NiO and has shown good agreement with experimental photoemission spectra and with the oxygen Kα X-ray emission spectrum.

https://iopscience.iop.org/article/10.1088/0953-8984/9/4/002/pdf

First-principles calculations of the electronic structure and spectra of strongly correlated systems: the LDA+ U method

Rapid progress in the synthesis and processing of materials with structure on nanometer length scales has created a demand for greater scientific understanding of thermal transport in nanoscale devices, individual nanostructures, and nanostructured materials. This review emphasizes developments in experiment, theory, and computation that have occurred in the past ten years and summarizes the present status of the field. Interfaces between materials become increasingly important on small length scales. The thermal conductance of many solid–solid interfaces have been studied experimentally but the range of observed interface properties is much smaller than predicted by simple theory. Classical molecular dynamics simulations are emerging as a powerful tool for calculations of thermal conductance and phonon scattering, and may provide for a lively interplay of experiment and theory in the near term. Fundamental issues remain concerning the correct definitions of temperature in nonequilibrium nanoscale systems. Modern Si microelectronics are now firmly in the nanoscale regime—experiments have demonstrated that the close proximity of interfaces and the extremely small volume of heat dissipation strongly modifies thermal transport, thereby aggravating problems of thermal management. Microelectronic devices are too large to yield to atomic-level simulation in the foreseeable future and, therefore, calculations of thermal transport must rely on solutions of the Boltzmann transport equation; microscopic phonon scattering rates needed for predictive models are, even for Si, poorly known. Low-dimensional nanostructures, such as carbon nanotubes, are predicted to have novel transport properties; the first quantitative experiments of the thermal conductivity of nanotubes have recently been achieved using microfabricated measurement systems. Nanoscale porosity decreases the permittivity of amorphous dielectrics but porosity also strongly decreases the thermal conductivity. The promise of improved thermoelectric materials and problems of thermal management of optoelectronic devices have stimulated extensive studies of semiconductor superlattices; agreement between experiment and theory is generally poor. Advances in measurement methods, e.g., the 3ω method, time-domain thermoreflectance, sources of coherent phonons, microfabricated test structures, and the scanning thermal microscope, are enabling new capabilities for nanoscale thermal metrology.

/pdf/nanoscale-thermal-transport-1frv881kzm.pdf

Nanoscale thermal transport

The MN+1AXN phases: A new class of solids

The conversion of heat to electricity by thermoelectric devices may play a key role in the future for energy production and utilization. However, in order to meet that role, more efficient thermoelectric materials are needed that are suitable for high-temperature applications. We show that the material system AgPb m SbTe 2+ m may be suitable for this purpose. With m = 10 and 18 and doped appropriately, n -type semiconductors can be produced that exhibit a high thermoelectric figure of merit material ZT max of ∼2.2 at 800 kelvin. In the temperature range 600 to 900 kelvin, the AgPb m SbTe 2+ m material is expected to outperform all reported bulk thermoelectrics, thereby earmarking it as a material system for potential use in efficient thermoelectric power generation from heat sources.

http://science.sciencemag.org/content/sci/303/5659/818.full.pdf

Cubic AgPbmSbTe2+m: Bulk Thermoelectric Materials with High Figure of Merit

Thermoelectric materials, capable of converting a thermal gradient to an electric field and vice versa, could be useful in power generation and refrigeration. But the fabrication of the available high-performance thermoelectric materials is not easily scaled up to the volumes needed for large-scale heat energy scavenging applications. Nanostructuring improves thermoelectric capabilities of some materials, but good thermoelectric materials tend not to take readily to nanostructuring. How about silicon? It can be processed on a large scale but has poor thermoelectric properties. Two groups now show that silicon's thermoelectric properties can be vastly improved by structuring it into arrays of nanowires and carefully controlling nanowire morphology and doping. So with more development, silicon may have potential as a thermoelectric material. Thermoelectric materials interconvert thermal gradients and electric fields for power generation or for refrigeration1,2. Thermoelectrics currently find only niche applications because of their limited efficiency, which is measured by the dimensionless parameter ZT—a function of the Seebeck coefficient or thermoelectric power, and of the electrical and thermal conductivities. Maximizing ZT is challenging because optimizing one physical parameter often adversely affects another3. Several groups have achieved significant improvements in ZT through multi-component nanostructured thermoelectrics4,5,6, such as Bi2Te3/Sb2Te3 thin-film superlattices, or embedded PbSeTe quantum dot superlattices. Here we report efficient thermoelectric performance from the single-component system of silicon nanowires for cross-sectional areas of 10 nm × 20 nm and 20 nm × 20 nm. By varying the nanowire size and impurity doping levels, ZT values representing an approximately 100-fold improvement over bulk Si are achieved over a broad temperature range, including ZT ≈ 1 at 200 K. Independent measurements of the Seebeck coefficient, the electrical conductivity and the thermal conductivity, combined with theory, indicate that the improved efficiency originates from phonon effects. These results are expected to apply to other classes of semiconductor nanomaterials.

Silicon nanowires as efficient thermoelectric materials

Thermoelectrics is an old field. In 1823, Thomas Seebeck discovered that a voltage drop appears across a sample that has a temperature gradient. This phenomenon provided the basis for thermocouples used for measuring temperature and for thermoelectric power generators. In 1838, Heinrich Lenz placed a drop of water on the junction of metal wires made of bismuth and antimony. Passing an electric current through the junction in one direction caused the water to freeze, and reversing the current caused the ice to quickly melt; thus thermoelectric refrigeration was demonstrated (figure 1).

Thermoelectric Materials: New Approaches to an Old Problem

Seebeck, electrical, and thermal conductivity data are reported on CoSb3, and doped and undoped alloys of Co1−x Ir x Sb3−y As y from 20 to 700 K. n‐type semiconductors were obtained by doping with Ni, Te, or Pd, and the hole concentration in p‐type samples was increased by substitution of Fe, Ru, Os, and Ge. An estimated maximum value for ZT of 0.6 (Z is the figure of merit) was found for a Te‐doped (n‐type) alloy at 700 K. For p‐type alloys, the maximum value of ZT was found to be 0.3 at 550 K. Electrical and thermal transport data also are reported for CoAs3, RhSb3, and IrSb3. Most of the samples investigated were polycrystalline, but a few measurements on CoSb3 single crystals also are discussed.

Thermoelectric properties of CoSb3 and related alloys

Thermomechanical cyclic response of an ultrafine-grained NiTi shape memory alloy

Atomic Displacement Parameters and the Lattice Thermal Conductivity of Clathrate-like Thermoelectric Compounds

Mg2Si1–xSnx compounds are low-cost and environmentally friendly thermoelectric materials expected to be applied as power generators in the intermediate temperature range. Optimization of the thermoelectric properties of Mg2Si1–xSnx compounds can be accomplished by the precise control and adjustment of the Mg content. A series of Mg2(1+z)Si0.5–ySn0.5Sby (0 ≤ y ≤ 0.015 and 0 ≤ z ≤ 0.15) compounds with controlled Mg content were synthesized by a two-step solid-state reaction method, followed by a spark plasma sintering technique. On the basis of optimized thermoelectric properties via doping with Sb, the effect of a variable content of Mg spanning from understoichiometry to overstoichiometry has been systematically explored. The results indicate that when the actual Mg content exceeds the stoichiometric amount, the dominant point defects in Mg2(1+z)Si0.49Sn0.5Sb0.01 compounds are interstitial Mg and Si/Sn vacancies. At the same time, the electron concentration is enhanced with increasing content of Mg. Howev...

Jeff Sharp

Papers

Thermoelectric Materials: New Approaches to an Old Problem

Thermoelectric properties of CoSb3 and related alloys

Thermomechanical cyclic response of an ultrafine-grained NiTi shape memory alloy

Atomic Displacement Parameters and the Lattice Thermal Conductivity of Clathrate-like Thermoelectric Compounds

Optimized Thermoelectric Properties of Sb-Doped Mg2(1+z)Si0.5–ySn0.5Sby through Adjustment of the Mg Content