Strong enhancement of phonon scattering through nanoscale grains in lead sulfide thermoelectrics

We present nanocrystalline PbS, which was prepared using a solvothermal method followed by spark plasma sintering, as a promising thermoelectric material. The effects of grains with different length scales on phonon scattering of PbS samples, and therefore on the thermal conductivity of these samples, were studied using transmission electron microscopy and theoretical calculations. We found that a high density of nanoscale grain boundaries dramatically lowered the thermal conductivity by effectively scattering long-wavelength phonons. The thermal conductivity at room temperature was reduced from 2.5 W m1K 1 for ingot-PbS (grain size 4200 lm) to 2.3 W m1K 1 for micro-PbS (grain size 40.4 lm); remarkably, thermal conductivity was reduced to 0.85 W m1 K 1 for nano-PbS (grain size B30 nm). Considering the full phonon spectrum of the material, a theoretical model based on a combination of first-principles calculations and semiempirical phonon scattering rates was proposed to explain this effective enhancement. The results show that the high density of nanoscale grains could cause effective phonon scattering of almost 61%. These findings shed light on developing high-performance thermoelectrics via nanograins at the intermediate temperature range.This contribution was supported primarily by the startup of the South University of Science and Technology of China, supported by the Shenzhen government, and the national 1000 plan for young scientists. This work was also partially supported by a grant-in-aid of ‘985 Project’ from Xi’an Jiaotong University, the National Natural Science Foundation of China (Grant No. 21201138 and 11204228), the National Basic Research Program of China (2012CB619402 and 2014CB644003) and the Fundamental Research Funds for the Central UniversitiesS

Lateral electrical transport, optical properties and photocurrent measurements in two-dimensional arrays of silicon nanocrystals embedded in SiO2

In this study we investigate the electronic transport, the optical properties, and photocurrent in two-dimensional arrays of silicon nanocrystals (Si NCs) embedded in silicon dioxide, grown on quartz and having sizes in the range between less than 2 and 20 nm. Electronic transport is determined by the collective effect of Coulomb blockade gaps in the Si NCs. Absorption spectra show the well-known upshift of the energy bandgap with decreasing NC size. Photocurrent follows the absorption spectra confirming that it is composed of photo-generated carriers within the Si NCs. In films containing Si NCs with sizes less than 2 nm, strong quantum confinement and exciton localization are observed, resulting in light emission and absence of photocurrent. Our results show that Si NCs are useful building blocks of photovoltaic devices for use as better absorbers than bulk Si in the visible and ultraviolet spectral range. However, when strong quantum confinement effects come into play, carrier transport is significantly reduced due to strong exciton localization and Coulomb blockade effects, thus leading to limited photocurrent