Industrial applications require the production of InN thin films with controlled epitaxy and good quality, i.e., uniformity and fine crystallinity, through a process of thin film deposition. In this context, InN has been previously deposited on Si(100), sapphire(0001), Al2O3 (0001) and 4H/6H-SiC (0001) substrates by using chemical vapour deposition (CVD), molecular beam epitaxy (MBE) and atomic-layer deposition (ALD) techniques, among others. The latter technique is particularly interesting for enabling a well-controlled growth with layer-by-layer formation, where the molecular precursors are inserted into the gas chamber at different time slots. Therefore, the lack of gas phase reactivity of the molecular sources would require that the major role leading to the thin film growth is played by surface-driven processes. In addition, the ALD technique employs lower temperatures that are beneficial for the crystal stability of InN, as it is wellknown that this material undergoes decomposition at temperature T starting from ~450 to up to 700 °C, depending on the methodology for growth. Trimethylindium (TMI) is a popular precursor for the In-rich layer formation in InN and In2O3 deposition. In the former case, Deminskyi et al. have demonstrated that the presence of carbon-based impurities, that are usually associated to the TMI precursor, could be significantly reduced upon use of ammonia (NH3) plasma as the nitrogen (N) precursor. The self-limiting chemistry for InN growth has been achieved at T= 320 °C, with deposition rate of 0.47 -0.51 Å/cycle, and an ALD window determined of T= 240 -260 °C. This step is assumed to release methane (CH4) through the reaction between the Hcontaining plasma (from NH3 decomposition) and chemisorbed methylindium (MI), which constitutes the presumed final point of the half-cycle towards the In-rich layer formation. The remaining NH2 radicals should then undergo chemisorption to form a NH2-terminated surface, whereas eventual NH radicals are not expected to be a frequent specimen at the conditions that are typical of an ALD experiment. In the next half-cycle, the TMI insertion into the gas chamber is primarily thought to lead to its physisorption onto the NH2-terminated surface, in which the dipole-dipole interaction occurs through the p-empty orbital (from TMI) and a lone pair (from NH2). Nonetheless, Hwang et al. have employed in situ-Raman spectroscopy to verify that the TMI decomposition in gas phase is feasible at T= 120 -535 °C, in N2 environment, in a process that is characterized by the homolytic dissociation into the MI precursor and CH3 radicals that quickly recombine into ethane (C2H6). The In-rich layer formation onto the NH2-terminated surface could then be achieved through a reaction mechanism involving the adsorption of i) TMI in an intact form, ii) dimethylindium (DMI) or iii) MI, where ii) and iii) involve precursor decomposition in gas phase. On the other hand, the surface-driven decomposition in i) exhibits lower activation barriers that should favor the deposition rate. Another precursor for ALD and conventional chemical vapor deposition (CVD) of In2O3, with potential use in InN deposition, is tris(N,N′-diisopropyl-2-dimethylamidoguanidinato (III) (ITG). This molecule pertains to a class of precursors where the indium atom (In) is surrounded by three bidentate ligands with In-N bonds. The idea is that the replacement of In-C bonds-from TMI-to weaker In-N bonds in the coordination sphere would facilitate the ligand decomposition and, ultimately, reduce the amount of carbon impurities. However, its use for InN deposition is considered more challenging, possibly due to its thermal instability in gas phase at lower temperatures. Buttera and collaborators have found that ITG should decompose in a two-step process: i) the ligand dechelation, in which one of the In-N bonds from the ligand is elongated and broken, as the ligand is rotated to allow the back-bone nitrogen group to form a coordination bond to the indium atom, and ii) the elimination of the carbodiimide (CDI) moiety, as the backbone dimethyl-nitrogen is transferred to the indium atom. While the dechelated intermediate was at higher free energy compared to the undecomposed precursor, the increased entropy when releasing the CDI molecule caused the second step to become so thermodynamically favorable that the decomposition was driven towards the products, at ALD conditions for temperature and pressure, indicating that the precursor would decompose in gas phase if left long enough.