<i>Ab initio</i>modeling of quantum transport properties of molecular electronic devices

TLDR

The authors present a self‑consistent ab initio method for modeling quantum transport in atomic‑scale nanoelectronic devices under bias. The method employs density functional theory with norm‑conserving nonlocal pseudopotentials and nonequilibrium Green’s functions, using a screening approximation to reduce the open system to a finite region and incorporating electrode interactions via self‑energies. Applied to single‑wall carbon nanotubes on Al electrodes, the technique overcomes first‑principles modeling challenges and shows two transmission eigenvectors yielding a ballistic conductance of roughly one quantum, about half the value of an ideal infinite nanotube.

Abstract

We report on a self-consistent ab initio technique for modeling quantum transport properties of atomic and molecular scale nanoelectronic devices under external bias potentials. The technique is based on density functional theory using norm conserving nonlocal pseudopotentials to define the atomic core and nonequilibrium Green's functions (NEGF's) to calculate the charge distribution. The modeling of an open device system is reduced to a calculation defined on a finite region of space using a screening approximation. The interaction between the device scattering region and the electrodes is accounted for by self-energies within the NEGF formalism. Our technique overcomes several difficulties of doing first principles modeling of open molecular quantum coherent conductors. We apply this technique to investigate single wall carbon nanotubes in contact with an Al metallic electrode. We have studied the current-voltage characteristics of the nanotube-metal interface from first principles. Our results suggest that there are two transmission eigenvectors contributing to the ballistic conductance of the interface, with a total conductance $G\ensuremath{\approx}{G}_{0}$ where ${G}_{0}{=2e}^{2}/h$ is the conductance quanta. This is about half of the expected value for infinite perfect metallic nanotubes.