In principle, this protocol is designed to reduce the experiment dimensionality to 1D, as it only considers the shortest path from apex of the tip to the sample no matter the tip shape, rather than considering the lateral extent of the growth. The use of such a protocol is supported by the fact that we often observed deposits much wider than the lift height despite not observing any deposition at slightly smaller pulse widths, as shown in SI-3 for all datapoints. Sweeping the lift height is done at the same spot on the substrate, with the substrate electrochemically cleaned between experiments through lifting of the substrate potential above the cobalt oxidation potential. In all cases lifting the potential resulted in the deposits dissolving, indirectly confirming that they consist of cobalt (SI-3). were done in a 50 mM CoSO4 (DMSO) solution (which is one order of magnitude lower than that used for the CV in Figure ). The substrate rest potential was empirically chosen to be right before cobalt deposition was observed with the STM (-700/-900 mV (circles, squares), and -850 mV/-1050 mV (diamonds) vs. Au QRE, respectively.). The tip rest potential was set 200 mV positive to that of the substrate to enable imaging. Given that the substrate is already almost at the required potential for cobalt reduction and that the potential difference between cobalt reduction and DMSO oxidation is found to be ~1.7 V, we estimate a required potential of 1.5 V for the tip.