Protective CrN-based coatings are of interest for applications requiring a combination of corrosion resistance and toughness. Here, the processing-microstructure-properties relationships for metallic Cr, binary CrN, and quaternary CrSiCN coatings are reported. Hexamethyldisilazane (HMDS) was used as a single-source organosilicon precursor for Si and C during plasma-enhanced magnetron sputtering (PEMS). By varying the availability of reactive species during coating growth, graded coating architectures were produced. Scanning and transmission electron microscopy revealed that as Si and C content increased, the coating microstructure evolved from a coarse, columnar growth structure (0 at.% Si), to a nanocolumnar structure (3 at.% Si), and, finally, to a dense, nanoscale structure (6 at.% Si). Coating surface topography was characterized using optical microscopy and atomic force microscopy. While the CrSiCN coating deposited at the highest HMDS flow rate exhibited the lowest nanoscale surface roughness (Rq = 6.74 nm), it also had the greatest area fraction of microscopic surface defects. Evidence of the formation of secondary Cr2N phases within the graded interlayers of the coatings was acquired from selected area electron diffraction analysis. However, the practical adhesion of the coatings, as evaluated by the Rockwell C indentation test, was not adversely affected. Nanoindentation testing revealed that greater incorporation of Si and C into the CrN-based coatings increased coating hardness from 25.4 ± 1.6 GPa to 30.7 ± 1.8 GPa and decreased apparent elastic modulus from 295 ± 14 GPa to 284 ± 12 GPa. Contact angle goniometry was conducted to determine the wettability of the coatings. It was found that sessile water contact angles decreased from 86.5° ± 1.6° to 77.3° ± 2.1° as coating Si and C content increased.
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