Mapping the site-specific potential energy landscape for chemisorbed and physisorbed aromatic molecules on the Si(1 1 1)-7 × 7 surface by time-lapse STM

Lock, Duncan; Sakulsermsuk, Sumet; Palmer, Richard E.; Sloan, Peter

doi:10.1088/0953-8984/27/5/054003

Cited by 19 publications

(24 citation statements)

References 31 publications

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“…Also, periodic DFT calculations [22] using a 2×2 mimic surface reported 1.2 eV chemisorption energy. However, new time-lapse STM experiments [28] indicate that the used pre-factor is too small and result in a chemisorption energy of 1.4 eV, well in line with our cluster calculations.…”

Section: Introductionsupporting

confidence: 88%

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Local resonances in STM manipulation of chlorobenzene on Si(111)-7×7: performance of different cluster models and density functionals

Utecht

Klamroth

2018

Molecular Physics

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Hot localised charge carriers on the Si(111)-7×7 surface are modelled by small charged clusters. Such resonances induce non-local desorption, i.e. more than 10 nm away from the injection site, of chlorobenzene in scanning tunnelling microscope experiments. We used such a cluster model to characterise resonance localisation and vibrational activation for positive and negative resonances recently. In this work, we investigate to which extent the model depends on details of the used cluster or quantum chemistry methods and try to identify the smallest possible cluster suitable for a description of the neutral surface and the ion resonances. Furthermore, a detailed analysis for different chemisorption orientations is performed. While some properties, as estimates of the resonance energy or absolute values for atomic changes, show such a dependency, the main findings are very robust with respect to changes in the model and/or the chemisorption geometry.

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Section: Introductionsupporting

confidence: 88%

“…We chose an adsorption site on the faulted half at a centre adatom and rest-atom position as the core of our model clusters. This adsorption site showed the highest reaction rates in previous experimental studies [28] and was therefore chosen to be investigated. We chose the same protocol for construction of the clusters as in Ref.…”

Section: Cluster Modelsmentioning

confidence: 99%

Local resonances in STM manipulation of chlorobenzene on Si(111)-7×7: performance of different cluster models and density functionals

Utecht

Klamroth

2018

Molecular Physics

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“…. The found chemisorption energy of ≈1.6 eV compares well to time lapse STM‐experiments performed later on, which reported ≈1.4 eV. In Ref.…”

Section: Introductionmentioning

confidence: 70%

Desorption induced by low energy charge carriers on Si(111)‐7 × 7: First principles molecular dynamics for benzene derivates

2018

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We use clusters for the modeling of local ion resonances caused by low energy charge carriers in STM‐induced desorption of benzene derivates from Si(111)‐7 × 7. We perform Born–Oppenheimer molecular dynamics for the charged systems assuming vertical transitions to the charged states at zero temperature, to rationalize the low temperature activation energies, which are found in experiment for chlorobenzene. Our calculations suggest very similar low temperature activation energies for toluene and benzene. For the cationic resonance transitions to physisorption are found even at 0 K, while the anion remains chemisorbed during the propagations. Further, we also extend our previous static quantum chemical investigations to toluene and benzene. In addition, an in depth analysis of the ionization potentials and electron affinities, which are used to estimate resonance energies, is given. © 2018 Wiley Periodicals, Inc.

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“…For each nonlocal atomic-manipulation experiment a large STM image was recorded with passive parameters (no molecular displacement) [31] of a surface partly covered with chemisorbed toluene molecules which appear as dark-spots, see figure 3(a). The tip was positioned at the centre of the image and a current injection performed with set voltage, current and time (here +2.8 V, 750 pA and 10 s).…”

Section: Stm Induced Nonlocal Atomic Manipulationmentioning

confidence: 99%

Common source of light emission and nonlocal molecular manipulation on the Si(111)−7 × 7 surface

et al. 2019

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The tip of a scanning tunnelling microscope can inject hot electrons into a surface with atomic precision. Their subsequent dynamics and eventual decay can result in atomic manipulation of an adsorbed molecule, or in light emission from the surface. Here, we combine the results of these two near identical experimental techniques for the system of toluene molecules chemisorbed on the Si(111)−7×7 surface at room temperature. The radial dependence of molecular desorption away from the tip injection site conforms to a two-step ballistic-diffusive transport of the injected hot electrons across the surface, with a threshold bias voltage of +2.0 V. We find the same threshold voltage of +2.0 V for light emission from the bare Si(111)−7×7 surface. Comparing these results with previous published spectra we propose that both the manipulation (here, desorption or diffusion) and the light emission follow the same hot electron dynamics, only differing in the outcome of the final relaxation step which may result in either molecular displacement, or photon emission.

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Mapping the site-specific potential energy landscape for chemisorbed and physisorbed aromatic molecules on the Si(1 1 1)-7 × 7 surface by time-lapse STM

Cited by 19 publications

References 31 publications

Local resonances in STM manipulation of chlorobenzene on Si(111)-7×7: performance of different cluster models and density functionals

Local resonances in STM manipulation of chlorobenzene on Si(111)-7×7: performance of different cluster models and density functionals

Desorption induced by low energy charge carriers on Si(111)‐7 × 7: First principles molecular dynamics for benzene derivates

Common source of light emission and nonlocal molecular manipulation on the Si(111)−7 × 7 surface

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