Conduction mechanisms in biphenyl dithiol single-molecule junctions

Bürkle, M. and Viljas, J. K. and Vonlanthen, D. and Mishchenko, A. and Schön, G. and Mayor, M. and Wandlowski, T. and Pauly, F.. (2012) Conduction mechanisms in biphenyl dithiol single-molecule junctions. Physical Review B, Vol. 85, H. 7 , 075417.

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Official URL: http://edoc.unibas.ch/dok/A6031590

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Based on density-functional theory calculations, we report a detailed study of the single-molecule charge-transport properties for a series of recently synthesized biphenyl-dithiol molecules. The torsion angle ϕ between the two phenyl rings, and hence the degree of π conjugation, is controlled by alkyl chains and methyl side groups. We consider three different coordination geometries, namely, top-top, bridge-bridge, and hollow-hollow, with the terminal sulfur atoms bound to one, two, and three gold surface atoms, respectively. Our calculations show that different coordination geometries give rise to conductances that vary by one order of magnitude for the same molecule. Irrespective of the coordination geometries, the charge transport calculations predict a cos2ϕ dependence of the conductance, which is confirmed by our experimental measurements. We demonstrate that the calculated transmission through biphenyl dithiols is typically dominated by a single transmission eigenchannel formed from π electrons. For perpendicular orientation of the rings a residual conductance arises from σ-π couplings. But only for a single molecule with a completely broken conjugation we find a nearly perfect degeneracy of the σ-π eigenchannels for the hollow-hollow-type contact in our theory.
Faculties and Departments:05 Faculty of Science > Departement Chemie > Chemie > Molecular Devices and Materials (Mayor)
UniBasel Contributors:Mayor, Marcel and Vonlanthen, David
Item Type:Article, refereed
Article Subtype:Research Article
Publisher:American Institute of Physics
Note:Publication type according to Uni Basel Research Database: Journal article
Identification Number:
Last Modified:08 Nov 2012 16:23
Deposited On:08 Nov 2012 16:17

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