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An effective strategy for improving the charge transport efficiency of p-type Cu 2 O photocathodes is the use of counter n-type semiconductors with a proper band alignment, preferably using Al-doped ZnO (AZO). Atomic layer deposition (ALD)-prepared AZO films show an increase in the built-in potential at the Cu 2 O/AZO interface as well as an excellent conformal coating with a thin thickness on irregular Cu 2 O. Considering the thin thickness of the AZO overlayers, it is expected that the composition of the Al and the layer stacking sequence in the ALD process will significantly influence the charge transport behavior and the photoelectrochemical (PEC) performance. We designed various stacking orders of AZO overlayers where the stacking layers consisted of Al 2 O 3 (or Al) and ZnO using the atomically controlled ALD process. Al doping in ZnO results in a wide bandgap and does not degrade the absorption efficiency of Cu 2 O. The best PEC performance was obtained for the sample with an AZO overlayer containing conductive Al layers in the bottom and top regions. The Cu 2 O/AZO/TiO 2 /Pt photoelectrode with this overlayer exhibits an open circuit potential of 0.63 V and maintains a high cathodic photocurrent value of approximately -3.2 mA cm -2 at 0 V RHE for over 100 min.

Optimal n-Type Al-Doped ZnO Overlayers for Charge Transport Enhancement in p-Type Cu2O Photocathodes