Physics of large thermoelectric power factors in SnSe nanoflakes in mid-temperature range.

We have theoretically investigated the underlying physics of observed high electrical conductivity (σ), simultaneous increase of σ and Seebeck coefficient (S) with temperature, and large power factors (PFs) in nominally undoped SnSe nanoflakes sintered at different temperatures, reported recently in Mandavaet al(2022Nanotechnology33155710). Given the fact that S and σ show unusual temperature trends and that the undoped SnSe samples are highly porous and disordered, the conventional Boltzmann theory does not appear to be an appropriate model to describe their transport properties. We have, instead, used a strong disorder model based on percolation theory where charge and energy transport take place through hopping between localized states to understand these observations. Our model is able to explain the observed temperature dependence of σ and S with temperature. Large σ can be explained by a high density of localized states and a large hopping rate. The sample sintered at a higher temperature has lower disorder (σDOS) and higher hopping rate (1/τ0). We findσDOS= 0.151 eV and 1/τ0= 0.143 × 1015s-1for sample sintered at 673 K andσDOS= 0.044 eV and 1/τ0= 2.023 × 1015s-1for sample sintered at 703 K. These values are comparable to the reported values of transition frequencies, confirming that the dominant charge transport mechanism in these SnSe nanoflakes is hopping transport. Finally, we suggest that hopping transport via localized states can result in enhanced thermoelectric properties in disordered polycrystalline materials.

Probing the path for achieving a broad temperature plateau of the figure of merit in thermoelectric nanocomposite materials.

The efficiency of a thermoelectric device depends directly on the average figure of merit (zT) of the material. A high average zT requires a broad temperature plateau with a high zT, but state-of-the-art thermoelectric materials display a peaked zT over a narrow temperature range due to a strong temperature dependence of transport properties. In this work, using Boltzmann transport theory, we systematically investigate the underlying physics and propose a strategy for attaining a broad temperature plateau of zT through proper engineering of the interfacial barrier height in PbTe nanocomposite material. The optimized barrier height (U constantzT) not only enhances the zT but also maintains its high value over a wide temperature range [Tmin :Tmax ]. It has been found that for p = 2.8 × 1020 cm-3, the U constantzT is 0.112 eV at which zT varies between 1.9-2.14 over a wide temperature range of 550-850 K, resulting in a high average zT of 2.02 in comparison to a bulk value of 1.22. Also, for p = 5 × 1019 cm-3, UconstantzT is 0.102 eV at which zT varies between 1.046-1.435 for a temperature range of 300-600K, resulting in a high average zT of 1.27 over a bulk value of 0.844. The above results show that the range [Tmin :Tmax ] depends on carrier concentration which, in turn, determines the position of the Fermi level (Ef ) and Fermi window at Tmin and Tmax . To obtain a broad temperature plateau of zT, the findings show that at Tmin, Ef should lie inside the band and zT should show strong variation with barrier height, whereas at Tmax , Ef should lie in the band gap and zT should have little variation with barrier height. This trend allows us to choose UconstantzT which synergistically optimizes the transport properties at Tmin with Tmax to give a broad temperature plateau of zT. This work proposes a new advantage of interfacial scattering which enhances the average zT and also provides necessary guidelines to experimentalists for synthesizing a highly efficient thermoelectric device.

Tailoring of Seebeck coefficient with surface roughness effects in silicon sub-50-nm films.

The effect of surface roughness on the Seebeck coefficient in the sub-50-nm scale silicon ultra thin films is investigated theoretically using nonequilibrium Green's function formalism. For systematic studies, the surface roughness is modelled by varying thickness periodically with square wave profile characterized by two parameters: amplitude (A 0) and wavelength (λ). Since high Seebeck coefficient is obtained if the temperature difference between the ends of device produces higher currents and higher induced voltages, we investigate how the generated current and induced voltage is affected with increasing A 0 and λ. The theoretical investigations show that pseudoperiodicity of the device structure gives rise to two effects: firstly the threshold energy at which the transmission of current starts is shifted towards higher energy sides and secondly transmission spectra of current possess pseudobands and pseudogaps. The width of the pseudobands and their occupancies determine the total generated current. It is found that current decreases with increasing A 0 but shows a complicated trend with λ. The trends of threshold energy determine the trends of Seebeck voltage with roughness parameters. The increase in threshold energy makes the current flow in higher energy levels. Thus, the Seebeck voltage, i.e. voltage required to nullify this current, increases. Increase in Seebeck voltage results in increase in Seebeck coefficient. We find that threshold energy increases with increasing A 0 and frequency (1/λ). Hence, Seebeck voltage and Seebeck coefficient increase vice versa. It is observed that Seebeck coefficient is tuneable with surface roughness parameters.