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Lissau H, Frisenda R, Olsen ST, et al. Tracking molecular resonance forms of donor-acceptor push-pull molecules by single-molecule conductance experiments. Nat Commun. 2015;6:10233doi: 10.1038/ncomms10233.
Lissau, H., Frisenda, R., Olsen, S. T., Jevric, M., Parker, C. R., Kadziola, A., Hansen, T., van der Zant, H. S., Brøndsted Nielsen, M., & Mikkelsen, K. V. (2015). Tracking molecular resonance forms of donor-acceptor push-pull molecules by single-molecule conductance experiments. Nature communications, 610233. https://doi.org/10.1038/ncomms10233
Lissau, Henriette, et al. "Tracking molecular resonance forms of donor-acceptor push-pull molecules by single-molecule conductance experiments." Nature communications vol. 6 (2015): 10233. doi: https://doi.org/10.1038/ncomms10233
Lissau H, Frisenda R, Olsen ST, Jevric M, Parker CR, Kadziola A, Hansen T, van der Zant HS, Brøndsted Nielsen M, Mikkelsen KV. Tracking molecular resonance forms of donor-acceptor push-pull molecules by single-molecule conductance experiments. Nat Commun. 2015 Dec 15;6:10233. doi: 10.1038/ncomms10233. PMID: 26667583; PMCID: PMC4682163.
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Nat Commun. 2015 Dec 15;6:10233. doi: 10.1038/ncomms10233.

Tracking molecular resonance forms of donor-acceptor push-pull molecules by single-molecule conductance experiments.

Nature communications

Henriette Lissau, Riccardo Frisenda, Stine T Olsen, Martyn Jevric, Christian R Parker, Anders Kadziola, Thorsten Hansen, Herre S J van der Zant, Mogens Brøndsted Nielsen, Kurt V Mikkelsen

Affiliations

  1. Department of Chemistry, University of Copenhagen, Universitetsparken 5, Copenhagen DK-2100, Denmark.
  2. Kavli Institute of Nanoscience, Delft University of Technology, GA Delft 2600, The Netherlands.

PMID: 26667583 PMCID: PMC4682163 DOI: 10.1038/ncomms10233

Abstract

The ability of molecules to change colour on account of changes in solvent polarity is known as solvatochromism and used spectroscopically to characterize charge-transfer transitions in donor-acceptor molecules. Here we report that donor-acceptor-substituted molecular wires also exhibit distinct properties in single-molecule electronics under the influence of a bias voltage, but in absence of solvent. Two oligo(phenyleneethynylene) wires with donor-acceptor substitution on the central ring (cruciform-like) exhibit remarkably broad conductance peaks measured by the mechanically controlled break-junction technique with gold contacts, in contrast to the sharp peak of simpler molecules. From a theoretical analysis, we explain this by different degrees of charge delocalization and hence cross-conjugation at the central ring. Thus, small variations in the local environment promote the quinoid resonance form (off), the linearly conjugated (on) or any form in between. This shows how the conductance of donor-acceptor cruciforms is tuned by small changes in the environment.

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