“…Originally demonstrated by Pd metallisation of am ercaptopyridine SAM on Au(111), the scheme has been extended to different metals (e.g.,P d, Pt, Au, Rh), different coordinating moieties (-SH, thiazoleo ramino), and SAMs of differentm olecular architectures. [14,[16][17][18][19][20][21][22][23][24][25][26][27][28] Determined by am olecular property insteado f ad efect in the SAM, the coordination mediated deposition scheme not only provides routine access to metal/SAM/metal sandwich structures but also offers new opportunities for metal deposition on SAMsi ncluding bimetallic systems through the combined deposition of coordinated metal and metal from the bulk electrolyte. [25,29] Even though variousm etalsh ave been successfully deposited on top of different SAMs by employing the coordination controlled scheme, the underlying mechanism and the factors controlling metal nucleation and growth at the outer SAM interface remainl argely unclear.T his is highlighted by the morphologyo ft he metal deposits for which both two-dimensional monoatomic-heighti slands [14, 19, 22-24, 27, 28] and three-dimensional particles af ew nanometres in size [18,25,26] have been reported, but the cause of the differences in morphology are not understood.…”