Vacuum-Referred Binding Energies of Bismuth and Lanthanide Levels in ARE(Si,Ge)O<sub>4</sub> (A = Li, Na; RE = Y, Lu): Toward Designing Charge-Carrier-Trapping Processes for Energy Storage
Tianshuai Lyu, P. Dorenbos
Abstract
<p>Developing a feasible design principle for solid-state materials for persistent luminescence and storage phosphors with high charge carrier storage capacity remains a crucial challenge. Here we report a methodology for such rational design via vacuum referred binding energy (VRBE) diagram aided band structure engineering and crystal synthesis optimization. The ARE(Si,Ge)O<sub>4</sub> (A = Li, Na; RE = Y, Lu) crystal system was selected as a model example. Low-temperature (10 K) photoluminescence excitation and emission spectra of bismuth- and lanthanide-doped ARE(Si,Ge)O<sub>4</sub> system were first systematically studied, and the corresponding VRBE schemes were then established. Guided by these VRBE schemes, Bi<sup>3+</sup> afterglow and storage phosphor properties were explored in NaLu<sub>1-x</sub>Y<sub>x</sub>GeO<sub>4</sub>. By combining Bi<sup>3+</sup> with Bi<sup>3+</sup> itself or Eu<sup>3+</sup>, Bi<sup>3+</sup> appears to act as a deep hole-trapping center, while Bi<sup>3+</sup> and Eu<sup>3+</sup> act as less-deep electron traps. Trap depth tunable afterglow and storage were realized in NaLu<sub>1-x</sub>Y<sub>x</sub>GeO<sub>4</sub>:0.01Bi<sup>3+</sup> and NaLu<sub>1-x</sub>Y<sub>x</sub>GeO<sub>4</sub>:0.01Bi<sup>3+</sup>,0.001Eu<sup>3+</sup> by adjusting x, leading to conduction band engineering. More than 28 h of persistent luminescence of Bi<sup>3+</sup> was measurable in NaYGeO<sub>4</sub>:0.01Bi<sup>3+</sup> due to electron release from Bi<sup>2+</sup> and recombination with a hole at Bi<sup>4+</sup>. The charge carrier storage capacity in NaYGeO<sub>4</sub>:0.01Bi<sup>3+</sup> was discovered to increase ∼7 times via optimizing synthesis condition at 1200 °C during 24 h. The thermoluminescence (TL) intensity of the optimized NaYGeO<sub>4</sub>:0.001Bi<sup>3+</sup> and NaYGeO<sub>4</sub>:0.01Bi<sup>3+</sup>,0.001Eu<sup>3+</sup> is ∼3, and ∼7 times higher than the TL of the state-of-the-art X-ray storage phosphor BaFBr(I):Eu. Proof-of-concept color tuning for anti-counterfeiting application was demonstrated by combining the discovered and optimized NaYGeO<sub>4</sub>:0.01Bi<sup>3+</sup> afterglow phosphor with perovskite CsPbBr<sub>3</sub> and CdSe quantum dots. Information storage application was demonstrated by UV-light- or X-ray-charged NaYGeO<sub>4</sub>:0.01Bi<sup>3+</sup>,0.001Eu<sup>3+</sup> phosphor dispersed in a silicone gel imaging film. This work not only reports excellent storage phosphors but more importantly provides a design principle that can initiate more exploration of afterglow and storage phosphors in a designed way through combining VRBE-scheme-guided band structure engineering and crystal synthesis optimization.</p>