Computational Chemistry for Molecular Electronics
P. S. Krstica, D. J. Dean
,
, a,
X. -G. Zhanga,
D. Kefferb,
Y. S. Lengc
P. T. Cummingsc, d
J. C. Wellse
aPhysics Division, Oak Ridge National Laboratory, Oak Ridge, TN 37831, USA.
bDepartment of Chemical Engineering, University of Tennessee, Knoxville, TN, 37996-2200, USA.
cDepartment of Chemical Engineering, Vanderbilt University, Nashville, TN 37235-1604, USA.
dChemical Sciences Division, Oak Ridge National
Laboratory, Oak Ridge, TN 37831, USA.
eComputer Science and Mathematics Division, Oak Ridge National
Laboratory, Oak Ridge, TN 37831, USA
Abstract
We present a synergetic effort of a group of theorists to characterize a molecular
electronics device through a multiscale modeling approach. We combine electronic-structure
calculations with molecular dynamics and Monte Carlo simulations to predict the structure of
self-assembled molecular monolayers on a metal surface. We also develop a novel insight into
molecular conductance, with a particular resolution of its fundamental channels, which stresses
the importance of a complete molecular structure description of all components of the system,
including the leads, the molecule, and their contacts. Both molecular dynamics and electron
transport simulations imply that knowledge of detailed molecular structure and system geometry
are critical for successful comparison with carefully performed experiments. We illustrate our
findings with benzenedithiolate molecules in contact with gold.
Author Keywords: molecular electronic, conductance, SAM formation, MD, DFT
Corresponding author.