Superlattices in the Pb–Tl–O system with layer thicknesses in the 4–6 nm range were electrodeposited from a single aqueous solution by pulsing the applied potential during deposition. The current‐time transients that resulted from the potential steps were monitored to both calculate and tailor the composition profiles of the superlattices during growth. The Cottrell method was used to determine that Tl(l) oxidation was diffusion limited at high potentials. The diffusion limitation resulted in a composition profile that was graded throughout the layer with a t−1/2 dependence. Superlattices grown at lower potentials in which both reactants were under kinetic control had square composition profiles.

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