Quantum and classical thermoelectric transport in quantum dot nanocomposites

Abstract

Quantum dot nanocomposites are potentially high-efficiency thermoelectric materials, which could outperform superlattices and random nanocomposites in terms of manufacturing cost-effectiveness and material properties because of the reduction of thermal conductivity due to the phonon-interface scattering, the enhancement of Seebeck coefficient due to the formation of minibands, and the enhancement of electrical conductivity due to the phonon-bottleneck effect in electron-phonon scattering for quantum-confined electrons. In this paper, we investigate the thermoelectric transport properties of quantum dot nanocomposites through a two-channel transport model that includes the transport of quantum-confined electrons through the hopping mechanism and the semiclassical transport of bulk-like electrons. For the quantum-confined electrons whose wave functions are confined in the quantum dots with overlapping tail extending to the matrix, we develop a tight-binding model together with the Kubo formula and the Green’s function method to describe the transport processes of these electrons. The formation of minibands due to the quantum confinement and the phonon-bottleneck effect on carrier-phonon scattering are considered. For transport of bulk-like electrons, a Boltzmann-transport–equation-based semiclassical model is used to describe the multiband transport processes of carriers. The intrinsic carrier scatterings as well as the carrier-interface scattering of these bulk-like electrons are considered. We then apply the two-channel transport model to predict thermoelectric transport properties of n-type PbSe/PbTe quantum dot nanocomposites with PbSe quantum dots uniformly embedded in the PbTe matrix. The dependence of thermoelectric transport coefficients on the size of quantum dots, interdot distance, doping concentration, and temperature are studied in detail. Due to the formation of minibands and the phonon-bottleneck effect on carrier-phonon scattering, we show that simultaneous enhancement of electrical conductivity and Seebeck coefficient can be realized in quantum dot nanocomposites. Our study could shed some light on the design of high-efficiency thermoelectric materials for energy conversion and thermal management.