Driven Liouville von Neumann Approach for Time-Dependent Electronic Transport Calculations in a Nonorthogonal Basis-Set Representation

A nonorthogonal localized basis-set
implementation of the driven
Liouville von Neumann (DLvN) approach is presented. The method is
based on block-orthogonalization of the Hamiltonian and overlap matrix
representations, yielding nonoverlapping blocks that correspond to
the various system sections. An extended Hückel description
of gold/benzene-dithiol/gold and gold/pyridine-dithiol/gold junctions
is used to demonstrate the performance of the method. The presented
generalization is an important milestone toward using the DLvN approach
for performing accurate dynamic electronic transport calculations
in realistic model systems, based on density functional theory packages
that rely on atom-centered basis-set representations.