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In this paper, the atomic layer deposition (ALD) of ultra-thin films (<4 nm) of $Al_{2}O_{3}$ and $HfO_{2}$ on Au-supported monolayer (1L) $MoS_{2}$ is investigated, providing an insight on the nucleation mechanisms in the early stages of the ALD process. A preliminary multiscale characterization of large area 1L-$MoS_{2}$ exfoliated on sputter-grown Au/Ni films revealed an almost conformal $MoS_{2}$ membrane with the Au topography and the occurrence of strain variations at the nanoscale. Ab-initio DFT calculations of $MoS_{2}$/Au(111) interface showed a significant influence of the Au substrate on the $MoS_{2}$ energy band structure, whereas small differences were accounted for the adsorption of the $H_{2}O$, TMA and TDMAHf precursors. This suggests a crucial role of nanoscale morphological effects, such as local curvature and strain of the $MoS_{2}$ membrane, in the enhanced physisorption of the precursors. Therefore, the nucleation and growth of $Al_{2}O_{3}$ and $HfO_{2}$ films onto 1L-$MoS_{2}$/Au was investigated, by monitoring the surface coverage as a function of the number (N) of ALD cycles, with N from 10 to 120. At low N values, a slower growth rate of the initially formed nuclei was observed for $HfO_{2}$, probably due to the bulky nature of the TDMAHf precursor as compared to TMA. On the other hand, the formation of continuous films was obtained in both cases for N>80 ALD cycles, corresponding to 3.6 nm $Al_{2}O_{3}$ and 3.1 nm $HfO_{2}$. Current mapping by C-AFM showed, for the same applied bias, a uniform insulating behavior of $Al_{2}O_{3}$ and the occurrence of few localized breakdown spots in the case of $HfO_{2}$, associated to less compact films regions. Finally, an increase of the 1L-$MoS_{2}$ tensile strain was observed by Raman mapping after encapsulation with both high-k films, accompanied by a reduction in the PL intensity., Comment: 26 pages, 9 figures

In this work, the nucleation and growth mechanism of aluminum oxide (Al2O3) in the early stages of the direct atomic layer deposition (ALD) on monolayer epitaxial graphene (EG) on silicon carbide (4H-SiC) has been investigated by atomic force microscopy (AFM) and Raman spectroscopy. Contrary to what is typically observed for other types of graphene, a large and uniform density of nucleation sites was observed in the case of EG and ascribed to the presence of the buffer layer at EG/SiC interface. The deposition process was characterized by Al2O3 island growth in the very early stages, followed by the formation of a continuous Al2O3 film (2.4 nm thick) after only 40 ALD cycles due to the islands coalescence, and subsequent layer-by-layer growth. Raman spectroscopy analyses showed low impact of the ALD process on the defects density and doping of EG. The EG strain was also almost unaffected by the deposition in the regime of island growth and coalescence, whereas a significant increase was observed after the formation of a compact Al2O3 film. The obtained results can have important implications for device applications of epitaxial graphene requiring the integration of ultra-thin high-k insulators., Comment: 19 pages, 6 figures