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Initiating and imaging the coherent surface dynamics of charge carriers in real space

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  • K. R. Rusimova

    (Centre for Nanoscience and Nanotechnology, University of Bath
    Nanoscale Physics Research Laboratory, School of Physics and Astronomy, University of Birmingham)

  • N. Bannister

    (Centre for Nanoscience and Nanotechnology, University of Bath)

  • P. Harrison

    (Centre for Nanoscience and Nanotechnology, University of Bath)

  • D. Lock

    (Centre for Nanoscience and Nanotechnology, University of Bath)

  • S. Crampin

    (Centre for Nanoscience and Nanotechnology, University of Bath)

  • R. E. Palmer

    (Nanoscale Physics Research Laboratory, School of Physics and Astronomy, University of Birmingham)

  • P. A. Sloan

    (Centre for Nanoscience and Nanotechnology, University of Bath)

Abstract

The tip of a scanning tunnelling microscope is an atomic-scale source of electrons and holes. As the injected charge spreads out, it can induce adsorbed molecules to react. By comparing large-scale ‘before’ and ‘after’ images of an adsorbate covered surface, the spatial extent of the nonlocal manipulation is revealed. Here, we measure the nonlocal manipulation of toluene molecules on the Si(111)-7 × 7 surface at room temperature. Both the range and probability of nonlocal manipulation have a voltage dependence. A region within 5–15 nm of the injection site shows a marked reduction in manipulation. We propose that this region marks the extent of the initial coherent (that is, ballistic) time-dependent evolution of the injected charge carrier. Using scanning tunnelling spectroscopy, we develop a model of this time-dependent expansion of the initially localized hole wavepacket within a particular surface state and deduce a quantum coherence (ballistic) lifetime of ∼10 fs.

Suggested Citation

  • K. R. Rusimova & N. Bannister & P. Harrison & D. Lock & S. Crampin & R. E. Palmer & P. A. Sloan, 2016. "Initiating and imaging the coherent surface dynamics of charge carriers in real space," Nature Communications, Nature, vol. 7(1), pages 1-7, November.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms12839
    DOI: 10.1038/ncomms12839
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    Cited by:

    1. Pieter J. Keenan & Rebecca M. Purkiss & Tillmann Klamroth & Peter A. Sloan & Kristina R. Rusimova, 2024. "Measuring competing outcomes of a single-molecule reaction reveals classical Arrhenius chemical kinetics," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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