M. Paulsson, T. Frederiksen, and M. Brandbyge
Molecular electronics: insight from first-principles transport simulations
CHIMIA 64, 350-355 (2010)
Conduction properties of nanoscale contacts can be studied using first-principles simulations. Such calculations give insight into details behind the conductance that is not readily available in experiments. For example, we may learn how the bonding conditions of a molecule to the electrodes affect the electronic transport. Here we describe key computational ingredients and discuss these in relation to simulations for scanning tunneling microscopy (STM) experiments with C60 molecules where the experimental geometry is well characterized. We then show how molecular dynamics simulations may be combined with transport calculations to study more irregular situations, such as the evolution of a nanoscale contact with the mechanically controllable break-junction technique. Finally we discuss calculations of inelastic electron tunnelling spectroscopy as a characterization technique that reveals information about the atomic arrangement and transport channels.
M. Brandbyge, T. Frederiksen, and M. Paulsson
DFT-NEGF approach to current-induced forces, vibrational signals, and heating in nanoconductors
Book chapter in T. Seideman Ed.
Current-Driven Phenomena in Nanoelectronics.
In this chapter we first introduce the DFT-NEGF method, which combines density
functional theory (DFT) with the nonequilibrium Green's function (NEGF) method in order
to treat atomic-scale conductors in the presence of current. We introduce the concept of
conductance eigenchannels within DFT-NEGF as a means of analysis of the elastic
conduction process. We then describe how the inelastic processes involving interaction
with vibrations can be calculated efficiently using DFT-NEGF and further approximations.
We show how these methods can be used to investigate how the electronic current can heat
the vibrations in the atomic-scale conductors and conclude with a discussion of some
current experiments in which this is observed.
L. Vitali, R. Ohmann, K. Kern, A. Garcia-Lekue, T. Frederiksen, D. Sánchez-Portal, and A. Arnau
Surveying molecular vibrations during the formation of metal-molecule nanocontacts
Nano Lett. 10, 657-660 (2010)
Molecular junctions have been characterized to determine the influence of the metal contact formation in the electron transport process through a single molecule. With inelastic electron tunneling spectroscopy and first-principles calculations, the vibration modes of a carbon monoxide molecule have been surveyed as a function of the distance from a copper electrode with unprecedented accuracy. We observe a continuous but nonlinear blue shift of the frustrated rotation mode in tunneling with decreasing distance followed by an abrupt softening upon contact formation. This indicates that the presence of the metal electrode sensibly alters the structural and conductive properties of the junction even without the formation of a strong chemical bond.
C. R. Arroyo, T. Frederiksen, G. Rubio-Bollinger, M. Vélez, A. Arnau, D. Sánchez-Portal, and N. Agraït
Characterization of single-molecule pentanedithiol junctions by inelastic electron
tunneling spectroscopy and first-principles calculations
Phys. Rev. B 81, 075405 (2010) [arXiv:1001.2392v1]
We study pentanedithiol molecular junctions formed by means of the break-junction technique with a scanning tunneling microscope at low temperatures. Using inelastic electron tunneling spectroscopy and first-principles calculations, the response of the junction to elastic deformation is examined. We show that this procedure makes a detailed characterization of the molecular junction possible. In particular, our results indicate that tunneling takes place through just a single molecule.