Using nonlocal empirical pseudopotentials, we compute the band structure and shear deformation potentials of strained Si, Ge, and SiGe alloys. Fitting the theoretical results to experimental data on the phonon‐limited carrier mobilities in bulk Si and Ge, the dilatation deformation potential Ξd is found to be 1.1 eV for the Si Δ minima, −4.4 eV for the Ge L minima, corresponding to a value for the valence band dilatation deformation potential a of approximately 2 eV for both Si and Ge. The optical deformation potential d0 is found to be 41.45 and 41.75 eV for Si and Ge, respectively. Carrier mobilities in strained Si and Ge are then evaluated. The results show a large enhancement of the hole mobility for both tensile and compressive strain along the [001] direction, but only a modest enhancement (approximately 60%) of the electron mobility for tensile biaxial strain in Si. Finally, from a fit to carrier mobilities in relaxed SiGe alloys, the effective alloy scattering potential is determined to be about 0...

Band structure, deformation potentials, and carrier mobility in strained Si, Ge, and SiGe alloys

Half-Heusler (HH) compounds have gained ever-increasing popularity as promising high temperature thermoelectric materials. High figure of merit zT of ≈1.0 above 1000 K has recently been realized for both n-type and p-type HH compounds, demonstrating the realistic prospect of these high temperature compounds for high efficiency power generation. Here, recent progress in advanced fabrication techniques and the intrinsic atomic disorders in HH compounds, which are linked to the understanding of the electrical transport, is discussed. Thermoelectric transport features of n-type ZrNiSn-based HH alloys are particularly emphasized, which is beneficial to further improving thermoelectric performance and comprehensively understanding the underlying mechanisms in HH thermoelectric materials. The rational design and realization of new high performance p-type Fe(V,Nb)Sb-based HH compounds are also demonstrated. The outlook for future research directions of HH thermoelectric materials is also discussed.

High Efficiency Half-Heusler Thermoelectric Materials for Energy Harvesting

Electron and phonon transport characteristics determines the potential of thermoelectric materials for power generation or refrigeration. This work shows that, different from most of high performance thermoelectric materials with dominant acoustic phonon scattering, the promising ZrNiSn based half-Heusler thermoelectric solid solutions exhibit an alloy scattering dominated charge transport. A low deformation potential and a low alloy scattering potential are found for the solid solutions, which is beneficial to maintain a relatively high electron mobility despite of the large effective mass, and can be intrinsic favorable features contributing to the noticeably high power factors of ZrNiSn based alloys. A quantitive description of the different phonon scattering mechanisms suggests that the point defect scattering is the most important mechanism that determines the phonon transport process of the solid solutions. The present results indicate that alloying can be an effective approach for such materials systems to enhance thermoelectric figure of merit ZT by reducing phonon thermal conductivity, while minimizing the deterioration of charge mobility due to the low alloy scattering potential.

Beneficial Contribution of Alloy Disorder to Electron and Phonon Transport in Half-Heusler Thermoelectric Materials

Forming solid solutions has long been considered an effective approach for good thermoelectrics because the lattice thermal conductivities are lower than those of the constituent compounds due to phonon scattering from disordered atoms. However, this effect could also be compensated by a reduction in carrier mobility due to electron scattering from the same disorder. Using a detailed study of n-type (PbTe)_(1–x) (PbSe)_x solid solution (0 ≤ x ≤ 1) as a function of composition, temperature, and doping level, quantitative modeling of transport properties reveals the important parameters characterizing these effects. Based on this analysis, a general criterion for the improvement of zT due to atomic disorder in solid solutions is derived and can be applied to several thermoelectric solid solutions, allowing a convenient prediction of whether better thermoelectric performance could be achieved in a given solid solution. Alloying is shown to be most effective at low temperatures and in materials that are unfavorable for thermoelectrics in their unalloyed forms: high lattice thermal conductivity (stiff materials with low Gruneisen parameters) and high deformation potential.

The Criteria for Beneficial Disorder in Thermoelectric Solid Solutions

The intrinsic structural disorder dramatically affects the thermal and electronic transport in semiconductors. Although normally considered an ordered compound, the half-Heusler ZrNiSn displays many transport characteristics of a disordered alloy. Similar to the (Zr,Hf)NiSn based solid solutions, the unsubstituted ZrNiSn compound also exhibits charge transport dominated by alloy scattering, as demonstrated in this work. The unexpected charge transport, even in ZrNiSn which is normally considered fully ordered, can be explained by the Ni partially filling interstitial sites in this half-Heusler system. The influence of the disordering and defects in crystal structure on the electron transport process has also been quantitatively analyzed in ZrNiSn1-xSbx with carrier concentration nH ranging from 5.0×1019 to 2.3×1021 cm−3 by changing Sb dopant content. The optimized carrier concentration nH ≈ 3–4×1020 cm−2 results in ZT ≈ 0.8 at 875K. This work suggests that MNiSn (M = Hf, Zr, Ti) and perhaps most other half-Heusler thermoelectric materials should be considered highly disordered especially when trying to understand the electronic and phonon structure and transport features.

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The intrinsic disorder related alloy scattering in ZrNiSn half-Heusler thermoelectric materials

The mean time between scattering due to a random alloy potential is considered. The development makes use of the Warren-Cowley order parameters and uses a pseudobinary alloy model for describing the arrangement of alloy concentrations on the allowed lattice sites. The resulting mean time between scattering is found to depend inversely on the square root of temperature and energy.

J. W. Harrison

Papers

Alloy scattering in ternary III-V compounds