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Real-time single-molecule imaging of quantum interference

An Erratum to this article was published on 06 August 2012

This article has been updated

Abstract

The observation of interference patterns in double-slit experiments with massive particles is generally regarded as the ultimate demonstration of the quantum nature of these objects. Such matter–wave interference has been observed for electrons1, neutrons2, atoms3,4 and molecules5,6,7 and, in contrast to classical physics, quantum interference can be observed when single particles arrive at the detector one by one. The build-up of such patterns in experiments with electrons has been described as the “most beautiful experiment in physics”8,9,10,11. Here, we show how a combination of nanofabrication and nano-imaging allows us to record the full two-dimensional build-up of quantum interference patterns in real time for phthalocyanine molecules and for derivatives of phthalocyanine molecules, which have masses of 514 AMU and 1,298 AMU respectively. A laser-controlled micro-evaporation source was used to produce a beam of molecules with the required intensity and coherence, and the gratings were machined in 10-nm-thick silicon nitride membranes to reduce the effect of van der Waals forces. Wide-field fluorescence microscopy detected the position of each molecule with an accuracy of 10 nm and revealed the build-up of a deterministic ensemble interference pattern from single molecules that arrived stochastically at the detector. In addition to providing this particularly clear demonstration of wave–particle duality, our approach could also be used to study larger molecules and explore the boundary between quantum and classical physics.

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Figure 1: Set-up for laser-evaporation, diffraction and nano-imaging of complex molecules.
Figure 2: Single-molecule imaging of PcH2 with subwavelength accuracy.
Figure 3: Build-up of quantum interference.
Figure 4: Comparison of interference patterns for PcH2 and F24PcH2.

Change history

  • 25 July 2012

    In the version of this Letter originally published, in Fig. 1c, the two white arrows were incorrectly positioned. This has now been corrected in the HTML and PDF versions.

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Acknowledgements

This project was funded by the FWF (contract FWF-Z149-N16; Wittgenstein) and the ESF/FWF EuroCore Program MIME (I146). The authors thank P. Geyer and P. Haslinger for building the in situ sputter cleaning apparatus, S. Deachapunya for his collaboration in testing the vapour pressures of PcH2, S. Nimmrichter for theory support and M. Tomandl for rendering Fig. 1. M.A. thanks W.E. Moerner for helpful discussions on single-molecule fluorescence. The chemical synthesis in Basel was supported by the ESF EuroCore Programme MIME (I146-N16), the Swiss National Science Foundation, and the NCCR ‘Nanoscale Science’.

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T.J. and M.A. conceived the experiments. T.J., A.M., M.Mu. and O.C. worked on the set-up of the experiment. T.J. performed the diffraction experiments. J.T. and M.Ma. designed and synthesized the F24PcH2 molecules. A.T. and O.C. fabricated the 10 nm diffraction gratings. P.A. developed the basis for the micro-evaporation source. M.A. and T.J. wrote the paper, with comments by all authors.

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Correspondence to Markus Arndt.

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Juffmann, T., Milic, A., Müllneritsch, M. et al. Real-time single-molecule imaging of quantum interference. Nature Nanotech 7, 297–300 (2012). https://doi.org/10.1038/nnano.2012.34

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