Advanced

Computational assignment of redox states to Coulomb blockade diamonds

Olsen, Stine T.; Arcisauskaite, Vaida; Hansen, Thorsten LU ; Kongsted, Jacob and Mikkelsen, Kurt V. (2014) In Physical Chemistry Chemical Physics 16(33). p.17473-17478
Abstract
With the advent of molecular transistors, electrochemistry can now be studied at the single-molecule level. Experimentally, the redox chemistry of the molecule manifests itself as features in the observed Coulomb blockade diamonds. We present a simple theoretical method for explicit construction of the Coulomb blockade diamonds of a molecule. A combined quantum mechanical/molecular mechanical method is invoked to calculate redox energies and polarizabilities of the molecules, including the screening effect of the metal leads. This direct approach circumvents the need for explicit modelling of the gate electrode. From the calculated parameters the Coulomb blockade diamonds are constructed using simple theory. We offer a theoretical tool for... (More)
With the advent of molecular transistors, electrochemistry can now be studied at the single-molecule level. Experimentally, the redox chemistry of the molecule manifests itself as features in the observed Coulomb blockade diamonds. We present a simple theoretical method for explicit construction of the Coulomb blockade diamonds of a molecule. A combined quantum mechanical/molecular mechanical method is invoked to calculate redox energies and polarizabilities of the molecules, including the screening effect of the metal leads. This direct approach circumvents the need for explicit modelling of the gate electrode. From the calculated parameters the Coulomb blockade diamonds are constructed using simple theory. We offer a theoretical tool for assignment of Coulomb blockade diamonds to specific redox states in particular, and a study of chemical details in the diamonds in general. With the ongoing experimental developments in molecular transistor experiments, our tool could find use in molecular electronics, electrochemistry, and electrocatalysis. (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Chemistry Chemical Physics
volume
16
issue
33
pages
17473 - 17478
publisher
Royal Society of Chemistry
external identifiers
  • wos:000341064800011
  • scopus:84905457600
ISSN
1463-9084
DOI
10.1039/c4cp02055c
language
English
LU publication?
yes
id
77017ec8-d607-4fcc-889e-0247af1da77e (old id 4717195)
date added to LUP
2014-10-31 09:15:43
date last changed
2017-08-20 04:11:42
@article{77017ec8-d607-4fcc-889e-0247af1da77e,
  abstract     = {With the advent of molecular transistors, electrochemistry can now be studied at the single-molecule level. Experimentally, the redox chemistry of the molecule manifests itself as features in the observed Coulomb blockade diamonds. We present a simple theoretical method for explicit construction of the Coulomb blockade diamonds of a molecule. A combined quantum mechanical/molecular mechanical method is invoked to calculate redox energies and polarizabilities of the molecules, including the screening effect of the metal leads. This direct approach circumvents the need for explicit modelling of the gate electrode. From the calculated parameters the Coulomb blockade diamonds are constructed using simple theory. We offer a theoretical tool for assignment of Coulomb blockade diamonds to specific redox states in particular, and a study of chemical details in the diamonds in general. With the ongoing experimental developments in molecular transistor experiments, our tool could find use in molecular electronics, electrochemistry, and electrocatalysis.},
  author       = {Olsen, Stine T. and Arcisauskaite, Vaida and Hansen, Thorsten and Kongsted, Jacob and Mikkelsen, Kurt V.},
  issn         = {1463-9084},
  language     = {eng},
  number       = {33},
  pages        = {17473--17478},
  publisher    = {Royal Society of Chemistry},
  series       = {Physical Chemistry Chemical Physics},
  title        = {Computational assignment of redox states to Coulomb blockade diamonds},
  url          = {http://dx.doi.org/10.1039/c4cp02055c},
  volume       = {16},
  year         = {2014},
}