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Mechanically controlled quantum interference in individual π-stacked dimers

Nature Chemistry volume 8, pages 1099–1104 (2016)Cite this article

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Abstract

Recent observations of destructive quantum interference in single-molecule junctions confirm the role of quantum effects in the electronic conductance properties of molecular systems. These effects are central to a broad range of chemical and biological processes and may be beneficial for the design of single-molecule electronic components to exploit the intrinsic quantum effects that occur at the molecular scale. Here we show that destructive interference can be turned on or off within the same molecular system by mechanically controlling its conformation. Using a combination of ab initio calculations and single-molecule conductance measurements, we demonstrate the existence of a quasiperiodic destructive quantum-interference pattern along the breaking traces of π-stacked molecular dimers. The results demonstrate that it is possible to control the molecular conductance over more than one order of magnitude and with a sub-ångström resolution by exploiting the subtle structure–property relationship of π-stacked dimers.

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Figure 1: Simulations of the electronic transport properties of S–OPE3 and S–OPE3–S.
Figure 2: Conductance analysis of S–OPE3 π-stacked dimers.
Figure 3: Statistical analysis of the conductance plateaus.
Figure 4: Statistical analysis of the conductance drops observed in single traces.

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Acknowledgements

The research leading to these results has received funding from the European Research Council (ERC) FP7 ERC Grant Agreement No. 240299 (Mols@Mols) and Horizon 2020 ERC Grant Agreement No. 648433.

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Author notes

  1. Riccardo Frisenda

    Present address: Present address: Instituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA-nanociencia), Campus de Cantoblanco, E-28049 Madrid, Spain,

Authors and Affiliations

  1. Kavli Institute of Nanoscience, Delft University of Technology, Lorentzweg 1, Delft, 2628 CJ, The Netherlands

    Riccardo Frisenda, Vera A. E. C. Janssen & Herre S. J. van der Zant

  2. Department of Chemical Engineering, Delft University of Technology, Julianalaan 136, Delft, 2628 BL, The Netherlands

    Ferdinand C. Grozema & Nicolas Renaud

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  1. Riccardo Frisenda
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Contributions

N.R. and F.C.G. performed the electronic transport calculations and the molecular dynamics simulations. R.F., V.A.E.C.J. and H.S.J.Z. performed the break-junction experiments. R.F. designed and implemented the analysis of the plateaus. N.R. designed and implemented the higher-order statistical analysis of conductance drops. All the authors wrote the manuscript.

Corresponding authors

Correspondence to Ferdinand C. Grozema or Herre S. J. van der Zant.

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The authors declare no competing financial interests.

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Frisenda, R., Janssen, V., Grozema, F. et al. Mechanically controlled quantum interference in individual π-stacked dimers. Nature Chem 8, 1099–1104 (2016). https://doi.org/10.1038/nchem.2588

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