Single‐Source Precursor Synthesis of a Compositionally Complex Early Transitional Metal Carbonitride (Ti,Zr,Hf,Nb,Ta)NₓC₁₋ₓ

Compositionally complex transitional metal nitrides are possible candidates for ultra‐high temperature usage and are known for their superior properties due to the high configuration entropy. It is often difficult to synthesize pure metal nitrides in bulk, due to significant oxygen contamination; hence, they are synthesized mainly as thin films through magnetron sputtering, chemical vapor deposition or surface nitridation of high entropy alloys. The present article reports on a single‐phase compositionally complex ceramic, i.e., (Ti₀.₂Zr₀.₂Hf₀.₂Nb₀.₂Ta₀.₂)NₓC₁₋ₓ, that is synthesized for the first time by employing an organometallic precursor route and using a double ammonolysis process. A multidisciplinary approach is performed to study these compositionally complex nitride and carbonitride systems, including experimental and theoretical investigations.