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.

We combine polarization-resolved low frequency Raman microscopy and dispersion-corrected density-functional calculations (DFT-D3) to study polymorph-dependent lattice vibrations in coronene, a model molecular system for nanographenes and disc-like organic semiconductors that exhibits two crystalline structures with distinct electronic and optical properties. Changes in low energy Raman-active lattice phonons are followed across the γ-to β-phase transition at 150 K. Raman frequencies calculated using DFT-D3 agree to within 4 cm −1 , and on the basis of polarisation dependence of peak positions and intensities we achieve a clear mode assignment. Studies of the associated atomic motions show how the pure librational and rotational modes of γ-coronene change into mixed roto-librations in the β-phase, explaining the remarkable differences in Raman spectra of the two phases.

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