Oxidation-reduction cycles (ORCs) on Au(111) in 0.1 M sulfuric acid solution change the electrode morphology due to the formation of many new nanosized islands. With increasing the cycle number, the roughness of the surface increases due to the formation of multiatomic-step adatom islands and pits. The final roughness value is a function of the applied potential window, number of ORCs, scan rate, electrolyte concentration, and any applied delay time. In a first experiment, the roughening was tracked by recording the STM images in 11 steps during 200 ORCs. The results show the formation of pyramidal islands and a linear correlation between the roughness amplitude and the cycle number. In a second experiment, the 200 cycles were studied in 38 steps, while after each step, two images were recorded with a 3 min delay by holding the potential in the double-layer window. This leads to a lower roughness increase due to the high surface mobility of the Au surface atoms, which smoothens the surface during the delay time. Finally, the oxidation-reduction charge density per cycle shows an inverse correlation with surface roughness due to the (111) terrace showing a higher surface oxidation charge than the other sites and facets. Each delay causes a strong increase in the oxidation charge which is a consequence of surface smoothening during the delays leading to an enhancement of the (111) related oxidation charge.
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