Methods for forming a transition metal nitride film on a substrate by atomic layer deposition and related semiconductor device structures are provided. In some embodiments, methods may include contacting a substrate with a first vapor phase reactant comprising a transition metal precursor and contacting the substrate with a second vapor phase reactant comprising an alkyl-hydrazine precursor. In some embodiments, related semiconductor device structures may include a PMOS transistor gate structure, the PMOS transistor gate structure including a transition metal nitride film and a gate dielectric between the transition nitride film and a semiconductor body. The transition metal nitride film includes a predominant (200) crystallographic orientation.