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Conductance measurements of a molecular wire, contacted between an epitaxialmolecule-metal bond and the tip of a scanning tunneling microscope, arereported. Controlled retraction of the tip gradually de-hybridizes the moleculefrom the metal substrate. This tunes the wire into the Kondo regime in whichthe renormalized molecular transport orbital serves as spin impurity at halffilling and the Kondo resonance opens up an additional transport channel.Numerical renormalization group simulations suggest this type of behavior to begeneric for a common class of metal molecule bonds. The results demonstrate anew approach to single-molecule experiments with atomic-scale contact controland prepare the way for the ab initio simulation of many-body transport throughsingle-molecule junctions.Comment: Main text: 41 pages including references and captions, 9 figures.  Supplementary information: 5 pages including 2 figures New experimental and  theoretical data supporting initial claims are added. The paper has been  reworked from the letter format into a longer versio

Kondo effect by controlled cleavage of a single-molecule contact