Atomic-level studies involving an electrochemical scanning tunneling microscope (EC-STM) flow-cell are presented. Multiple electrochemical atomic layer epitaxy (EC-ALE) cycles of CdTe formation were observed. For a binary compound (i.e., CdTe), an EC-ALE cycle involves exposure of the substrate to a solution of the first precursor (CdSO4), followed by exposure to the second precursor (TeO2), while maintaining potential control. Interleaving blank rinses may also be used, but were omitted in the present studies. To allow the exchange of solutions, the EC-STM cell was modified to allow solution exchange via a single peristaltic pump. A selection valve was used to choose the solution to be introduced into the cell. There is evidence that the growth of the initial layer of CdTe on Au(111), the (√7 × √7)-CdTe monolayer, can be improved in homogeneity and morphology by repeatedly depositing and stripping the Cd atomic layer. Therefore, a new starting cycle, which should improve the quality of deposits formed via EC-ALE, has been developed.