Among the prerequisites for the progress of single-molecule-based electronic devices are a better understanding of the electronic properties at the individual molecular level and the development of methods to tune the charge transport through molecular junctions. Scanning tunneling microscopy (STM) is an ideal tool not only for the characterization, but also for the manipulation of single atoms and molecules on surfaces. The conductance through a single molecule can be measured by contacting the molecule with atomic precision and forming a molecular bridge between the metallic STM tip electrode and the metallic surface electrode. The parameters affecting the conductance are mainly related to their electronic structure and to the coupling to the metallic electrodes. Here, the experimental and theoretical analyses are focused on single tetracenothiophene molecules and demonstrate that an in situ-induced direct desulfurization reaction of the thiophene moiety strongly improves the molecular anchoring by forming covalent bonds between molecular carbon and copper surface atoms. This bond formation leads to an increase of the conductance by about 50 % compared to the initial state.

Department of Nanoscale Science Max Planck Institute for Solid State Research Heisenbergstrasse 1 70569 Stuttgart Germany

Department of Organic Electronics Max Planck Institute for Solid State Research Heisenbergstrasse 1 70569 Stuttgart Germany

Institut de Physique École Polytechnique Fédérale de Lausanne EPFL SB IPHYS Direction Bâtiment PH Station 3 1015 Lausanne Switzerland

Institute of Applied Physics Technische Universität Braunschweig Mendelssohnstraße 2 38106 Braunschweig Germany

Institution Donostia International Physics Centre Paseo Manuel de Lardizabal 4 20018 Donostia San Sebastián Spain

Nanosurf Lab Institute of Physics of the Czech Academy of Science Cukrovarnicka 10 16253 Praha 6 Czech Republic

National Institute of Materials Physics Atomistilor Strasse No 405A 077125 Magurele Romania

Present address Institute of Applied Physics Technische Universität Braunschweig Mendelssohnstrasse 2 38106 Braunschweig Germany

Present address University of Cambridge Cavendish Laboratory J J Thomson Avenue Cambridge CB3 0HE UK

Present address University of Liverpool Department of Chemistry Crown Street Liverpool L69 7ZD UK

SUPA School of Physics and Astronomy University of St Andrews North Haugh St Andrews KY16 9SS UK

UPV EHU and Material Physics Center Centro Mixto CSIC UPV EHU Paseo Manuel de Lardizabal 5 20018 Donostia San Sebastián Spain

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Molecular sensitised probe for amino acid recognition within peptide sequences