Thermoelectric transport properties in nanoscale systems

Abstract

As the fast development of nanotechnology and further industrial applications, theoretical investigations upon nanoscale devices are in urgent need. Until now several formalisms have been well established in quantum transport of mesoscopic areas, including of tight-binding and first principle calculations. In this dissertation those methods were partly explored to explore transport and thermoelectric features in various models and actual devices.

The density functional theory plus non-equilibrium Green’s function serves well in the probing process of transport properties like conductance in mesoscopic systems. Atoms’ positions were treated as the only input parameters and one computation package based on NEGF-DFT loop was utilized to get the numerical results, then the corresponding thermal quantities were analysed.

The coherent transport exhibits an obvious character in transmission spectrum called transmission node, whose existence relies on the asymmetric structure of molecular junctions. In the main body of the thesis, firstly two types of model simulation were tested, and the following thermoelectric quantities showed that there’s one interesting signature in the thermopower performance, which was its temperature independence around transmission node. Through comparisons between different system parameters a rough regular pattern was obtained, that the degree of zero transmission and the energy difference around it influenced this temperature invariance feature at the same time. While these two properties were mainly determined by the natural structure of devices.

Besides model simulations the ab initio investigations were also carried out. Although the actual device was not easily altered as ideal models, some similar behaviours in the transmission and thermal curves were still found out. The temperature insensitivity was considered to appear more often in a π electron dominated molecular structure rather than ones with σ electron interactions.