Letter | Published:

Real-time single-molecule imaging of quantum interference

Nature Nanotechnology volume 7, pages 297300 (2012) | Download Citation

  • 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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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.

References

  1. 1.

    Elektroneninterferenzen an mehreren künstlich hergestellten Feinspalten. Z. Phys. 161, 454–474 (1961).

  2. 2.

    , , , & Single- and double-slit diffraction of neutrons. Rev. Mod. Phys. 60, 1067–1073 (1988).

  3. 3.

    , , & Diffraction of atoms by a transmission grating. Phys. Rev. Lett. 61, 1580–1583 (1988).

  4. 4.

    & Young's double-slit experiment with atoms: a simple atom interferometer. Phys. Rev. Lett. 66, 2689–2692 (1991).

  5. 5.

    & Nondestructive mass selection of small van der Waals clusters. Science 266, 1345–1348 (1994).

  6. 6.

    et al. Wave–particle duality of C60 molecules. Nature 401, 680–682 (1999).

  7. 7.

    , & Quantum reflection of He2 several nanometers above a grating surface. Science 331, 892–894 (2011).

  8. 8.

    The most beautiful experiment in physics. Phys. World 15, 15–17 (September 2002).

  9. 9.

    The double-slit experiment; available at (2002).

  10. 10.

    , & On the statistical aspect of electron interference phenomena. Am. J. Phys. 44, 306–307 (1976).

  11. 11.

    , , , & Demonstration of single-electron buildup of an interference pattern. Am. J. Phys. 57, 117–120 (1989).

  12. 12.

    , & in Quantum Mechanics Vol. 3, Ch. 1 (Addison Wesley, 1965).

  13. 13.

    et al. Wave and particle in molecular interference lithography. Phys. Rev. Lett. 103, 263601 (2009).

  14. 14.

    , , & Atomic wave diffraction and interference using temporal slits. Phys. Rev. Lett. 77, 4–7 (1996).

  15. 15.

    , & Time-resolved diffraction and interference: Young's interference with photons of different energy as revealed by time resolution. Phil. Trans. R. Soc. A 360, 1039–1059 (2002).

  16. 16.

    et al. Attosecond double-slit experiment. Phys. Rev. Lett. 95, 040401 (2005).

  17. 17.

    et al. The simplest double slit: interference and entanglement in double photoionization of H2. Science 318, 949–952 (2007).

  18. 18.

    et al. Direct observation of Young's double-slit interferences in vibrationally resolved photoionization of diatomic molecules. Proc. Natl Acad Sci. USA 108, 7302–7306 (2011).

  19. 19.

    et al. Localization and loss of coherence in molecular double-slit experiments. Nature Phys. 4, 649–655 (2008).

  20. 20.

    , & Quantum interference experiments with large molecules. Am. J. Phys. 71, 319–325 (2003).

  21. 21.

    & Principles of Optics (Pergamon Press, 1993).

  22. 22.

    et al. Alternating-gradient focusing and deceleration of large molecules. Phys. Rev. A 77, 031404R (2008).

  23. 23.

    et al. Slow beams of massive molecules. Eur. Phys. J. D 46, 307–313 (2007).

  24. 24.

    et al. Quantum interference of large organic molecules. Nature Commun. 2, 263 (2011).

  25. 25.

    , & Experimental challenges in fullerene interferometry. J. Mod. Opt. 47, 2811–2821 (2000).

  26. 26.

    , , , & Vibration induced electric dipole in a weakly bound molecular complex. Phys. Rev. Lett. 89, 253001 (2002).

  27. 27.

    et al. Influence of conformational molecular dynamics on matter wave interferometry. Phys. Rev. A 81, 031604 (2010).

  28. 28.

    & Optical detection and spectroscopy of single molecules in a solid. Phys. Rev. Lett. 62, 2535–2538 (1989).

  29. 29.

    & Breaking the diffraction resolution limit by stimulated emission: stimulated-emission-depletion fluorescence microscopy. Opt. Lett. 19, 780–782 (1994).

  30. 30.

    , & Single-molecule high-resolution imaging with photobleaching. Proc. Natl Acad. Sci. USA 101, 6462–6465 (2004).

  31. 31.

    et al. A Kapitza–Dirac–Talbot–Lau interferometer for highly polarizable molecules. Nature Phys. 3, 711–715 (2007).

  32. 32.

    , , , & Determination of atom–surface van der Waals potentials from transmission-grating diffraction intensities. Phys. Rev. Lett. 83, 1755–1758 (1999).

  33. 33.

    et al. Wave and particle in molecular interference lithography. Phys. Rev. Lett. 103, 263601 (2009).

  34. 34.

    , , & Diffraction of complex molecules by structures made of light. Phys. Rev. Lett. 87, 160401 (2001).

  35. 35.

    , , , & New prospects for de Broglie interferometry. Found. Phys. 42, 98–110 (2010).

  36. 36.

    , , , & Quantum interference of clusters and molecules. Rev. Mod. Phys. 84, 157–173 (2012).

  37. 37.

    , & An efficient two-step synthesis of metal-free phthalocyanines using a Zn(II) template. Chem. Commun. 1970–1971 (2009).

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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’.

Author information

Affiliations

  1. Vienna Center of Quantum Science and Technology, Faculty of Physics, University of Vienna, Boltzmanngasse 5, 1090 Vienna, Austria

    • Thomas Juffmann
    • , Adriana Milic
    • , Michael Müllneritsch
    • , Peter Asenbaum
    •  & Markus Arndt
  2. The Center for Nanoscience and Nanotechnology, Tel Aviv University, 69978 Tel Aviv, Israel

    • Alexander Tsukernik
    •  & Ori Cheshnovsky
  3. Department of Chemistry, University of Basel, St. Johannsring 19, 4056 Basel, Switzerland

    • Jens Tüxen
    •  & Marcel Mayor
  4. Karlsruhe Institute of Technology, Institute for Nanotechnology, PO Box 3640, 76021 Karlsruhe, Germany

    • Marcel Mayor
  5. School of Chemistry, The Raymond and Beverly Sackler faculty of exact sciences, Tel Aviv University, 69978 Tel Aviv, Israel

    • Ori Cheshnovsky

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Contributions

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.

Competing interests

The authors declare no competing financial interests.

Corresponding author

Correspondence to Markus Arndt.

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DOI

https://doi.org/10.1038/nnano.2012.34

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