Based on experimental obtained EI-MS fragments (Figure † and Table †) and reported decomposition pathways of comparable guanidinate ligand containing precursors in the literature, . The elimination of NMe2 fragments is calculated by taking HNMe2 and H2 as references while the elimination of the CN fragment is calculated by using HCN and H2 as references. The loss of NMe2 ligands from the precursor can be either NMe2 bound to CDI (pathway I) or NMe2 directly bound to Zr (pathway II). The computed energy costs for these NMe2 elimination steps are +1.12 eV for pathway I and +2.63 eV for pathway II. This difference arises from the change in Zr coordination after NMe2 elimination. In pathway I, Zr maintains its full coordination, while in pathway II, Zr coordination is lower since a Zr-N bond is removed. After the first step of NMe2 elimination, the precursor will continue losing carbodiimide (CDI) and CH3CH3CH2 (iPr) fragments. Finally, after losing another HNMe2 fragment in pathway I and a HCN fragment in pathway II, ZrN is formed using the selected precursor (1, Figure ). The computed overall reaction for both pathways is endothermic, indicating that the decomposition of selected SSP will not happen at room temperature and only begins at elevated temperatures. The experimental operating temperature for optimized ZrN growth was found to be 750 °C. Overall, the intermediates calculated in pathway I possess a lower reaction energy compared to the ones in pathway II, hinting that the intermediates in I are more stable. In addition, pathway I is arguably more likely, as the precursor is forming an imido species upon decomposition, that was experimentally found in EI-MS decomposition studies of a comparable gadolinium guanidinate precursor. Thin film analysis -Structure and crystallinity. Optimized process parameters were: substrate temperature from 550 °C to 850 °C, precursor evaporation temperature of 135 °C, nitrogen carrier gas flow of 100 sccm, pressure of 1 mbar. The influence of substrate temperature for ZrN films grown on Si and GC were investigated by means of XRD (Figure ) and b)) as well as Raman spectroscopy (Figure †) of the material on GC. The onset of crystallization was found to be 650 °C at which the (200) reflex of rock salt ZrN phase (PDF pattern no. 00-031-1493) was observed. Similarly, at 750 °C, solely the (200) reflex was obtained, but with a significantly increased intensity and narrow width indicating a higher degree of crystallinity as well as a higher thickness. The XRD pattern of the film grown at 850 °C shows reflexes corresponding to the (111) and (220) plane of rock salt ZrN accompanied by a broad (200) reflex with a high intensity hinting an enhanced crystallinity but less oriented growth. Additionally, the broad reflex shape indicates the presence randomly oriented ZrN crystal domains which could be embedded in an amorphous carbide matrix, hinted by the enhanced C content in the film as described later in (Table ). Comparison of the grain sizes estimated by the Scherrer equation confirms the temperature dependency and showcases the influence of the underlying substrate on the growth characteristics. While for the films grown on Si at 750 °C the largest grain sizes were calculated to be 25.5 nm, at 850 °C and 650 °C smaller grains with diameters of 12.4 nm and 7.4 nm were estimated, respectively. A similar trend was observed on GC, where the largest grains were obtained for the 750 °C sample with a diameter of 32.2 nm, followed by 17.9 nm for 850 °C and 10.9 nm for 650 °C. Overall, the grain sizes on GC are larger compared to Si at all temperatures, which could be explained by a different nucleation behaviour due to differences in surface energies leading to formation of larger grains. The Raman spectrum of the film on GC depicted in Figure † reveal three peaks corresponding to ZrN. From ~130 cm -1 to 250 cm -1 a broad scattering peak corresponding to overlapping of the transverse acoustic phonon (TA) and the longitudinal acoustic (LA) one. In addition, the asymmetric band (2A) appears at wavenumbers around 530 cm -1 . The broad appearance of the Raman peaks indicate the presence of N vacancies in the ZrN films. Again, the highest intensity Raman peaks were obtained for the films grown at 750 °C, supporting the results from XRD that at this deposition temperature, films with the highest degree of crystallinity were obtained.