Role of Paramagnetic Aluminum Hole Centers in UV–C Persistent Luminescence of Ca2Al2SiO7:Pr3+

IF 3.2 3区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry C Pub Date : 2024-12-13 DOI:10.1021/acs.jpcc.4c06848
Andris Antuzevics, Guna Krieke, Guna Doke, Pavels Rodionovs, Dace Nilova, Jekabs Cirulis, Andris Fedotovs, Uldis Rogulis
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Abstract

Materials with self-sustained emission in the ultraviolet (UV) spectral range present significant potential for practical applications. In this study, photochromic and persistent luminescence properties of Ca2Al2SiO7:Pr3+ are characterized by diffuse reflectance, photoluminescence, and thermally stimulated luminescence (TSL) spectroscopy methods. The material exhibits efficient persistent luminescence in the 250–350 nm range, with power density reaching 10.6 mW/m2 detected 10 s after 250 nm excitation and lasting for 3.7 h over the radiance threshold of 5 × 10–4 mW/m2/sr. In addition, photochromism is observed after either UV or X-ray irradiation. Multiple excitation cycles lead to noticeable coloration and reduced luminescence intensity, which can be restored by annealing. Electron paramagnetic resonance (EPR) spectroscopy indicates a correlation between persistent luminescence, photochromic properties, and paramagnetic centers in the material. The paramagnetic centers are identified as self-trapped holes at the Al(2) sites of the lattice, based on the g-factor and hyperfine interaction values determined from EPR and electron–nuclear double resonance (ENDOR) spectra simulations. These results provide a fundamental understanding of the structure–property relationship in Ca2Al2SiO7 and highlight practical considerations for developing UV–C persistent phosphor materials.

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顺磁铝孔中心在Ca2Al2SiO7:Pr3+紫外- c持续发光中的作用
在紫外线(UV)光谱范围内具有自持续发射的材料在实际应用中具有巨大的潜力。本研究采用漫反射、光致发光和热激发发光(TSL)光谱方法,对 Ca2Al2SiO7:Pr3+ 的光致变色和持续发光特性进行了表征。该材料在 250-350 纳米范围内表现出高效的持续发光特性,在 250 纳米激发 10 秒后检测到的功率密度达到 10.6 mW/m2,在 5 × 10-4 mW/m2/sr 的辐射阈值上可持续 3.7 小时。此外,在紫外线或 X 射线照射后还能观察到光致变色现象。多次激发会导致明显的褪色和发光强度降低,但退火后即可恢复。电子顺磁共振(EPR)光谱显示,持续发光、光致变色特性与材料中的顺磁中心之间存在关联。根据 EPR 和电子核双共振(ENDOR)光谱模拟确定的 g 因子和超细相互作用值,顺磁中心被确定为晶格 Al(2) 位点的自俘获空穴。这些结果提供了对 Ca2Al2SiO7 结构-性能关系的基本理解,并突出了开发紫外线-C 持久荧光粉材料的实际考虑因素。
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来源期刊
The Journal of Physical Chemistry C
The Journal of Physical Chemistry C 化学-材料科学:综合
CiteScore
6.50
自引率
8.10%
发文量
2047
审稿时长
1.8 months
期刊介绍: The Journal of Physical Chemistry A/B/C is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, and chemical physicists.
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