Preparation, electronic structure and photoluminescence properties of RE (RE = Ce, Yb)-activated SrAlSi4N7 phosphors

The electronic structure of SrAlSi4N7 was calculated using the CASTEP code and SrAlSi4N7 is an intermediate band gap semiconductor with an indirect energy gap of 3.6 eV. Ce3+ and Yb2+-activated SrAlSi4N7 samples were prepared by a solid-state reaction method at high temperature, and their photoluminescence properties were investigated. SrAlSi4N7:Ce3+ shows a broad band emission in the wavelength range of 450-700 nm, originating from the 5d(1)-4f(1) transition of Ce3+. The emission band of Ce3+ shifts to longer wavelength with an increase of Ce3+ concentration due to the increased Stokes shift and reabsorption by Ce3+. SrAlSi4N7:Yb2+ can be excited efficiently over a broad spectral range between 300 and 550 nm, and exhibits a single intense red emission at 600 nm with a full width at half maximum of 95 nm due to the electronic transitions from the excited state of 4f(13)5d to the ground state 4f(14) of Yb2+. The low energy of Yb2+ emission in SrAlSi4N7 can be attributed to the large nephelauxetic effect and crystal field splitting due to the coordination of Yb2+ by nitrogen. In addition, Sr1-2xCexLixAlSi4N7 shows higher thermal stability in air than that of Sr1-yYbyAlSi4N7 (0 <= x, y <= 0.1). A white-light LED can be generated by using single SrAlSi4N7:Ce3+ as the wavelength conversion phosphor combined with a blue LED chip (InGaN). The obtained LED exhibits a luminous efficiency of 74.3 lm W-1 at a corrected color temperature (CCT) up to 6350 K, and the color rendering index (CRI Ra) is around 78. These novel developed yellow-red phosphors have potential applications in spectral conversion materials for white-LEDs.