Photoluminescence and energy transfer of efficient and thermally stable white-emitting Ca9La(PO4)7:Ce3+, Tb3+, Mn2+ phosphors

The development of novel single-component white-emitting phosphors with high thermal stability is essential for improving the illumination quality of white light-emitting diodes. In this work, we synthesized a series of Ce³⁺, Tb³⁺, Mn²⁺ single- and multiple-doped Ca₉La(PO₄)₇ (CLPO) phosphors with β-Ca₃(PO₄)₂-type structure by the simple high-temperature solid-state reaction. The crystallization behavior, crystal structure, surface morphology, photoluminescence performance, decay lifetime and thermal stability were systematically investigated. The PL spectra and decay curves have evidenced the efficient energy transfer from Ce³⁺ to Tb³⁺ and from Ce³⁺ to Mn²⁺ in the CLPO host, and corresponding energy transfer efficiency reaches 41.8% and 54.1%, respectively. The energy transfer process of Ce³⁺→Tb³⁺ and Ce³⁺→Mn²⁺ can be deduced to the resonant type via dipole-dipole and dipole-quadrupole interaction mechanism, and corresponding critical distance were determined to be 12.23 and 14.4 Å, respectively. Based on the efficient energy transfer, the white light emission can be successfully achieved in the single-component CLPO:0.15Ce³⁺, 0.10Tb³⁺, 0.04Mn²⁺ phosphor, which owns CIE chromaticity coordinates of (0.3245, 0.3347), CCT of 5878 K, internal and external quantum efficiency of 84.51% and 69.32%. Especially, compared with the emission intensity at 25 °C, it still remains 98.5% at 150 °C and 92.0% at 300 °C. Based on these results, the single-component white light emission phosphor CLPO:0.15Ce³⁺, 0.10Tb³⁺, 0.04Mn²⁺ is a potential candidate for UV-converted white LEDs.