A new and efficient approach Using cleaving Of trimethylsilyl groups. to create covalent Au-C anchoring sites has been developed for single-molecule junction conductance measurements. Employing the mechanically controllable break junction (MCBJ) technique in liquid, we demonstrate the formation of highly conducting single molecular junctions of several opg derivatives.: The Created junctions are mechanically stable and exhibit. conductances around one order of magnitude higher than those of their dithiol analogues. Extended assembly and reaction times lead to oligomerization: Combined STM imaging and gap-mode Raman experiments provide,structure_evidence.to support the, formation;of.covalent Au-C contacts and further oligomerization.