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Two recent experimental (Li, J.~\emphj{et al}, \emph{Proc.\ Natl.\ Acad.\Sci.\ U.~S.~A.} {\bf 2014}, 111, 1282-1287) and theoretical studies (B\^aldea,I, \emph{Phys.\ Chem.\ Chem.\ Phys.}\ {\bf 2014}, 16, 25942-25949) haveaddressed the problem of tuning molecular charge and vibrational properties ofsingle molecules embedded in nanojunctions. These are molecular characteristicsescaping so far to an efficient experimental control in broad ranges. Here, wepresent a general argument demonstrating why, out of various experimentalplatforms possible, those wherein active molecules are asymmetrically coupledto electrodes are to be preferred to those symmetrically coupled for achievinga(n almost) complete redox process, and why electrochemical environment hasadvantages over "dry" setups. This study aims at helping to nanofabricatemolecular junctions using the most appropriate platforms enabling the broadestpossible bias-driven control of the redox state and vibrational modes of singlemolecules linked to electrodes.

An important impact of the molecule-electrode couplings asymmetry on the efficiency of bias-driven redox processes in molecular junctions