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Dynamic Effects on Electron Transport in Molecular Electronic Devices
KTH, School of Biotechnology (BIO), Theoretical Chemistry. (Yi Luo)
2010 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

HTML clipboardIn this thesis, dynamic effects on electron transport in molecular electronic devices are presented. Special attention is paid to the dynamics of atomic motions of bridged molecules, thermal motions of surrounding solvents, and many-body electron correlations in molecular junctions.

In the framework of single-body Green’s function, the effect of nuclear motions on electron transport in molecular junctions is introduced on the basis of Born-Oppenheimer approximation. Contributions to electron transport from electron-vibration coupling are investigated from the second derivative of current-voltage characteristics, in which each peak is corresponding to a normal mode of the vibration. The inelastic-tunneling spectrum is thus a useful tool in probing the molecular conformations in molecular junctions. By taking account of the many-body interaction between electrons in the scattering region, both time-independent and time-dependent many-body Green’s function formula based on timedependent density functional theory have been developed, in which the concept of state of the system is used to provide insight into the correlation effect on electron transport in molecular devices.

An effective approach that combines molecular dynamics simulations and first principles calculations has also been developed to study the statistical behavior of electron transport in electro-chemically gated molecular junctions. The effect of thermal motions of polar water molecules on electron transport at different temperatures has been found to be closely related to the temperature-dependent dynamical hydrogen bond network.

Place, publisher, year, edition, pages
Stockholm: KTH , 2010. , 67 p.
Series
Trita-BIO-Report, ISSN 1654-2312 ; 2010:6
Keyword [en]
molecular electronics
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-12676ISBN: 978-91-7415-604-1 (print)OAI: oai:DiVA.org:kth-12676DiVA: diva2:317895
Public defence
2010-06-09, FD41, Albanova University Center, Roslagstullsbacken, Stockholm, 10:00 (English)
Opponent
Supervisors
Note
QC20100630Available from: 2010-05-12 Created: 2010-05-05 Last updated: 2010-06-30Bibliographically approved
List of papers
1. Temperature-dependent statistical behavior of single molecular conductance in aqueous solution
Open this publication in new window or tab >>Temperature-dependent statistical behavior of single molecular conductance in aqueous solution
2008 (English)In: Journal of the American Chemical Society, ISSN 0002-7863, E-ISSN 1520-5126, Vol. 130, no 21, 6674-+ p.Article in journal (Refereed) Published
Abstract [en]

We have combined molecular dynamics simulations with first principles calculations to study electron 4 transport in a single molecule of perylene tetracarboxylic diimide (PTCDI) sandwiched between two gold electrodes with an aqueous electrolyte. This combination has for the first time allowed one to reveal statistical behavior of molecular conductance in solution at different temperatures and to produce conductance histograms that can be directly compared with experiments. Our calculations show that experimentally observed temperature-dependent conductance ran be attributed to the thermal effect on the hydrogen bonding network around the molecule and can be described by the radial distribution of water molecules surrounding the oxygen atom in the PTCDI molecule.

Keyword
JUNCTIONS, TRANSPORT
Identifiers
urn:nbn:se:kth:diva-12826 (URN)10.1021/ja8007648 (DOI)000256158200011 ()2-s2.0-44349181414 (Scopus ID)
Note
QC20100630Available from: 2010-05-12 Created: 2010-05-12 Last updated: 2017-12-12Bibliographically approved
2. Identification of switching mechanism in molecular junctions by inelastic electron tunneling spectroscopy
Open this publication in new window or tab >>Identification of switching mechanism in molecular junctions by inelastic electron tunneling spectroscopy
2008 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 112, no 29, 11018-11022 p.Article in journal (Refereed) Published
Abstract [en]

We present first-principles studies on electron transport properties of Pd-dithiolated oligoaniline-Pd molecular junctions. It is to demonstrate the possibility of using inelastic electron tunneling spectroscopy (IETS) to identify the switching mechanism in the molecular junction. Calculations have successfully reproduced the experimentally observed conductance switching behavior and the corresponding inelastic electron tunneling spectra. It is shown that the conductance switching is induced by conformation changes of the intercalated dithiolated oligoaniline in the junctions rather than oxidation/reduction as proposed earlier. Among three possible isomers, the low and high conductance states are related to two symmetrical structures. The possible involvement of asymmetric structure is discussed. It is revealed that chemical bonds between the terminal S atom and Pd electrodes are quite weak with relatively long bond distances.

Keyword
NEGATIVE DIFFERENTIAL RESISTANCE, SINGLE-MOLECULE, CONDUCTANCE, TRANSPORT, DEVICES, DENSITY
Identifiers
urn:nbn:se:kth:diva-12828 (URN)10.1021/jp800884g (DOI)000257724100062 ()2-s2.0-49149110910 (Scopus ID)
Note
QC20100630Available from: 2010-05-12 Created: 2010-05-12 Last updated: 2017-12-12Bibliographically approved
3. Field Effects on the Statistical Behavior of the Molecular Conductance in a Single Molecular Junction in Aqueous Solution
Open this publication in new window or tab >>Field Effects on the Statistical Behavior of the Molecular Conductance in a Single Molecular Junction in Aqueous Solution
2010 (English)In: NANO RES, ISSN 1998-0124, Vol. 3, no 5, 350-355 p.Article in journal (Refereed) Published
Abstract [en]

We have combined molecular dynamics simulations with first-principles calculations to study electron transport in a single molecular junction of perylene tetracarboxylic diimide (PTCDI) in aqueous solution under external electric gate fields. It is found that the statistics of the molecular conductance are very sensitive to the strength of the electric field. The statistics of the molecular conductance are strongly associated with the thermal fluctuation of the water molecules around the PTCDI molecule. Our simulations reproduce the experimentally observed three orders of magnitude enhancement of the conductance, as well as the temperature dependent conductance, under the electrochemical gates. The effects of the molecular polarization and the dipole rearrangement of the aqueous solution are also discussed.

Keyword
Molecular junction, field effect, solvent effect, temperature effect, statistical behavior, ELECTROCHEMICAL GATE, ELECTRON-TRANSPORT, CHARGE-TRANSPORT, MODULATION
Identifiers
urn:nbn:se:kth:diva-13843 (URN)10.1007/s12274-010-1038-9 (DOI)000278134800005 ()2-s2.0-77953021092 (Scopus ID)
Note
QC 20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2010-12-15Bibliographically approved
4. Conductance Oscillation in Dithiolated Oligoacene Junctions
Open this publication in new window or tab >>Conductance Oscillation in Dithiolated Oligoacene Junctions
(English)In: Journal of Physics: Condensed Matter, ISSN 0953-8984, E-ISSN 1361-648XArticle in journal (Refereed) Submitted
Identifiers
urn:nbn:se:kth:diva-13844 (URN)
Note
QC20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2017-12-12Bibliographically approved
5. Many-Body Interaction Formulism of Electron Transport in Molecular Junctions
Open this publication in new window or tab >>Many-Body Interaction Formulism of Electron Transport in Molecular Junctions
(English)Manuscript (preprint) (Other academic)
Identifiers
urn:nbn:se:kth:diva-13845 (URN)
Note
QC20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2010-06-30Bibliographically approved
6. Time-Dependent Current Through Molecular Junctions: Analysis in State Space
Open this publication in new window or tab >>Time-Dependent Current Through Molecular Junctions: Analysis in State Space
(English)Manuscript (preprint) (Other academic)
Identifiers
urn:nbn:se:kth:diva-13846 (URN)
Note
QC20100630Available from: 2010-06-30 Created: 2010-06-30 Last updated: 2010-06-30Bibliographically approved

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