Publication date: 15th December 2025
Transition metal nitrides are promising semiconductors for solar energy conversion and optoelectronics, offering narrower bandgaps and superior carrier transport compared to oxides. However, their synthetic complexity has limited exploration and led to poorly controlled defects. In this contribution, we use reactive co-sputtering to synthesize and engineer nanometer-scale nitride thin films with precise control over composition and doping in the Ti-Ta-N,[1] Zr-Ta-N,[2,3] and Hf-Ta-N systems. Starting from orthorhombic Ta3N5, we show that substitutional Ti doping improves photoconversion efficiency by modulating defect and recombination dynamics. While high Ti doping forms a secondary TiN phase, Zr and Hf yield tunable solid solutions in the Zr-Ta-N-(O) and Hf-Ta-N-(O) systems, exhibiting bandgap modulation and large refractive indices. Notably, a new bixbyite-type ternary compound, ZrTaN3, forms at a 1:1 Zr:Ta ratio, showing strong visible light absorption and photoanodic activity. DFT calculations reveal a tunable direct bandgap driven by cation ordering. These results underscore the potential of both established and emerging compositionally complex nitrides for solar energy and photonic applications, and highlight the importance of precise composition engineering to tune optoelectronic and charge transport characteristics.
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