Publication date: 21st July 2025
Tantalum nitride (Ta₃N₅) is a highly studied semiconductor for solar-driven water splitting. However, experimentally achieved efficiencies remain far below theoretical limits due to the formation of native and impurity defect states that impact charge carrier dynamics by facilitating trapping and recombination processes. In this study, we investigate the influence of different defect states in Ta₃N₅ thin films on ultrafast photocarrier dynamics using femtosecond transient absorption spectroscopy, as well as complementary photoluminescence and photoluminescence excitation measurements. Ta3N5 Photoelectrodes containing tailored shallow/deep defect state concentrations and structural disorder were synthesized by first sputtering TaOx, TaNx, and metallic Ta precursor films, followed by NH3 annealing. Through comparative studies of these samples, we identify and distinguish the important roles of both nitrogen vacancies and oxygen-related defects in shaping the charge carrier dynamics. Our results reveal that these defects function as efficient trapping and recombination centers for free carriers. The correlation with complementary measurements link shallow and deep defect properties with charge carrier dynamics and photoelectrochemical performance, enabling the tailored development of design strategies to overcome current limitations.
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