Oxygen vacancy-induced cerium self-reduction in cyan-emitting phosphors for high-quality white lighting and visible light communication applications
摘要
Self-reducing phosphors have attracted significant attention due to their avoidance of hazardous gases (H2/CO/N2), offering safer and more economical alternatives. This work reveals oxygen vacancy defect-induced Ce3+ self-reduction behavior in garnet structure. The Ca2Gd1−xZr2Al3O12:Ce3+ cyan phosphors were successfully synthesized via conventional high-temperature solid-state reaction in ambient atmosphere. Photoluminescence (PL) spectra revealed a strong emission centered at 490 nm, aligning well with the cyan component required in WLEDs. The relatively short fluorescence lifetime further implies the potential of CGZA:Ce3+/4+ phosphors for high-speed visible light communication (VLC). By combining electron paramagnetic resonance (EPR) spectroscopy with density functional theory (DFT) calculations, the self-reduction behavior of Ce4+ to Ce3+ in the garnet structure was elucidated. The results suggest that oxygen vacancies play a critical role in facilitating the reduction process. DFT calculations revealed that Ce doping significantly lowers the formation energy of oxygen vacancies, thereby promoting self-reduction. These findings provide valuable insights into the design of novel self-reducing Ce3+-based phosphors for advanced lighting and optical communication applications.
Graphical abstract