Initiating and imaging the coherent surface dynamics of charge carriers in real space.
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.
Centre for Nanoscience and Nanotechnology, Department of Physics, University of Bath, Bath BA2 7AY, UK.|Nanoscale Physics Research Laboratory, School of Physics and Astronomy, University of Birmingham, Birmingham B15 2TT, UK.
K R
KR
Rusimova
Centre for Nanoscience and Nanotechnology, Department of Physics, University of Bath, Bath BA2 7AY, UK.
N
N
Bannister
Centre for Nanoscience and Nanotechnology, Department of Physics, University of Bath, Bath BA2 7AY, UK.
P
http://orcid.org/0000-0001-9798-8710
P
Harrison
Centre for Nanoscience and Nanotechnology, Department of Physics, University of Bath, Bath BA2 7AY, UK.
D
D
Lock
Centre for Nanoscience and Nanotechnology, Department of Physics, University of Bath, Bath BA2 7AY, UK.
S
S
Crampin
Nanoscale Physics Research Laboratory, School of Physics and Astronomy, University of Birmingham, Birmingham B15 2TT, UK.
R E
RE
Palmer
Centre for Nanoscience and Nanotechnology, Department of Physics, University of Bath, Bath BA2 7AY, UK.
P A
PA
Sloan
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