Atomic-Level Structural and Electronic Properties of Hybrid Inorganic–Organic ZnO:Hydroquinone Superlattices Fabricated by ALD/MLD

We investigated crystalline ZnO:hydroquinone (HQ) superlattices grown layer-by-layer by the combined atomic/molecular layer deposition (ALD/MLD) technique; such ALD/MLD layer-engineered inorganic–organic thin films form a fundamentally new category of functional coherent hybrid materials that cannot be prepared by any other existing technique. Using quantum chemical methods, we derive atomic-level structural models for the ZnO:HQ superlattices and investigate their structural, spectroscopic, and electronic properties. By comparing the theoretical results with our experimental data we provide a detailed interpretation of experimentally measured infrared spectra, proving the presence of organic interfaces within the crystalline ZnO:HQ superlattices. We moreover show how the band structure of the hybrid material can be tailored by simple and experimentally feasible modifications of the organic constituent. The guidelines for the band-structure engineering of ZnO:HQ superlattices should be valuable for the systematic enhancement and exploitation of the functional properties of ALD/MLD-grown inorganic–organic superlattices and nanolaminates in general.