Conduction mechanisms in biphenyl dithiol single-molecule junctions

Bürkle, Marius; Viljas, Janne K.; Vonlanthen, David; Mishchenko, Artem; Schön, Gerd; Mayor, Marcel; Wandlowski, Thomas; Pauly, Fabian

Conduction mechanisms in biphenyl dithiol single-molecule junctions

Dateien

bürkle_211908.pdfGröße: 1.07 MBDownloads: 184

Datum

2012

Autor:innen

Bürkle, Marius

Viljas, Janne K.

Vonlanthen, David

Mishchenko, Artem

Schön, Gerd

Mayor, Marcel

Wandlowski, Thomas

Pauly, Fabian

Open Access-Veröffentlichung

Open Access Green

Sammlungen

Physik

Publikationstyp

Zeitschriftenartikel

Publikationsstatus

Published

Erschienen in

Physical Review B. 2012, 85(7). ISSN 1098-0121. eISSN 1550-235X. Available under: doi: 10.1103/PhysRevB.85.075417

Zusammenfassung

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 [ D. Vonlanthen et al. Angew. Chem., Int. Ed. 48 8886 (2009); A. Mishchenko et al. Nano Lett. 10 156 (2010)]. 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.

Fachgebiet (DDC)

530 Physik

Zitieren

ISO 690

BÜRKLE, Marius, Janne K. VILJAS, David VONLANTHEN, Artem MISHCHENKO, Gerd SCHÖN, Marcel MAYOR, Thomas WANDLOWSKI, Fabian PAULY, 2012. Conduction mechanisms in biphenyl dithiol single-molecule junctions. In: Physical Review B. 2012, 85(7). ISSN 1098-0121. eISSN 1550-235X. Available under: doi: 10.1103/PhysRevB.85.075417

BibTex

@article{Burkle2012Condu-21190,
  year={2012},
  doi={10.1103/PhysRevB.85.075417},
  title={Conduction mechanisms in biphenyl dithiol single-molecule junctions},
  number={7},
  volume={85},
  issn={1098-0121},
  journal={Physical Review B},
  author={Bürkle, Marius and Viljas, Janne K. and Vonlanthen, David and Mishchenko, Artem and Schön, Gerd and Mayor, Marcel and Wandlowski, Thomas and Pauly, Fabian}
}

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    <dcterms:abstract xml:lang="eng">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 [ D. Vonlanthen et al. Angew. Chem., Int. Ed. 48 8886 (2009); A. Mishchenko et al. Nano Lett. 10 156 (2010)]. 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.</dcterms:abstract>
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