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The thin layers of ZnO and ZnO: Al (Al doped zinc oxide—AZO) were deposited by the atomic deposition layer (ALD) method on silicon and glass substrates. The structures were deposited using diethylzinc (DEZ) and deionized water as zinc and oxygen precursors. A precursor of trimethylaluminum (TMA) was used to introduce the aluminum dopant. The present study of ALD-deposited ZnO and AZO films was motivated by their applications in photovoltaics. We attempted to expose several properties of such films. Structural, optical (including ellipsometric measurements) and electrical investigations were performed. We discussed the relations between samples doped with different Al fractions and their properties.