Electron and Spin Transport in Graphene-Based Nanodevices

Abstract: This thesis is devoted to the multi-scale modeling of electron and spin transport in graphene-based nanodevices. Several devices with fascinating structures and attractive properties have been designed by means of state-of-the-art computational methods, which include ab-initio molecular dynamics (MD) simulations for the geometry, density functional theory (DFT) for the electronic structure, and non-equilibrium Green’s functions (NEGF) for carriers transport properties.Poly-crystalline graphenes offer ample opportunities to make devices with desirable properties. We have systematically studied a type of poly-crystalline graphene constructed by zigzag and armchair graphene nanoribbons (ZGNR and AGNR). It is found that the choice of the supercells in modeling with periodic boundary conditions (PBC) has strong implications on the electronic and magnetic properties of such hybrid systems. A model with minimal lattice mismatch is obtained, which could be regarded as the most appropriate model for hybrid GNRs. With this model, it is revealed that the hybrid GNR is of ferromagnetism with a high Curie temperature. We have then designed armchair/zigzag graphene nanoribbon heterojunctions (AGNR|ZGNR) with a well-defined conductance oscillation and rectification behavior. It is shown that the resonance or nonresonance of the frontier orbitals between AGNR and ZGNR is the source of the oscillation and the asymmetric structure is the root of the rectification. A high rectification ratio can be achieved by tuning the width of ZGNR to enhance the asymmetric character of transmission function and to minimize the backward current.The electron transport properties of graphene can be modified by hydrogenation strips (HSs) formed from the absorbed hydrogen atoms. We have designed a new graphene nanoribbon that has zigzag-edged HSs placed at its middle region. It is found that the HS can electrically separate the GNR into sub-GNRs and each HS introduces two spin-polarized conducting edge-like states around the Fermi level. This leads to a significant enhancement of the conductance and the spinpolarization. We have also found that by introducing embedding a short sp3-edged section into the sp2-edged ZGNRs or a short sp2-edged section into the sp3-edged ZGNRs, the orbital symmetry mismatch between these two sections can induce the opening of the conductance energy gap in ZGNRs over a wide energy region. This simple strategy explains many unexplained experimental results and offers a simple strategy to design GNRs with a proper energy gap.We have also carefully examined the spin-polarization of chiral GNRs with reconstructed (2,1)-edges. It is found that the unsaturated (2,1)-edged chiral GNRs can possess strong current polarizations (nearly 100%) and a striking negative differential resistance (NDR) behavior.