MOE Laboratory of Bioinorganic and Synthetic Chemistry, KLGHEI of Environment and Energy Chemistry, School of Chemistry , Sun Yat-sen University , Guangzhou 510275 , China.
Beijing Synchrotron Radiation Facility, Institute of High Energy Physics , Chinese Academy of Sciences , Beijing 100039 , China.
Inorg Chem. 2018 Jul 16;57(14):8414-8421. doi: 10.1021/acs.inorgchem.8b01084. Epub 2018 Jun 26.
A detailed investigation on photoluminescence properties and energy transfer (ET) dynamics of Ce, Pr-doped BaYSiO is provided along with the potential X-ray excited luminescence application. The luminescence properties of Pr are studied in VUV-UV-vis spectral range at low temperature, and the spectral profiles of PrP and D emission lines are determined using time-resolved emission spectra. Upon 230 nm excitation, the electron population from Pr 4f5d state to its 4f excited state is discussed in detail. As Pr concentration rises, PrP and D luminescence possess different concentration-related properties. The incorporation of Ce in the codoped sample produces the strong Ce luminescence under 230 nm excitation, which is the combined result of Pr 4f5d → Ce 5d ET and Ce intrinsic excitation. On the other hand, the increasingly strong ET of Ce 5d → Pr 4f results in the decrease of Ce emission intensity and the gradual deviation of Ce luminescence decay from the single exponential in the system. By employing the Inokuti-Hirayama model, the dipole-dipole interaction is confirmed as the predominant multipolar effect in controlling this ET process, and the value of C is determined to be 9.97 × 10 m·s. Finally, the relatively low scintillation light yield of Ce-doped BaYSiO material impedes its application potential in the scintillator field, and the cosubstitution of Pr results in the observable decline of scintillation performance.
提供了关于 Ce、Pr 掺杂的 BaYSiO 光致发光特性和能量转移（ET）动力学的详细研究，以及其在 X 射线激发发光应用方面的潜力。在低温下，通过 VUV-UV-vis 光谱范围研究了 Pr 的发光特性，并通过时间分辨发射光谱确定了 PrP 和 D 发射线的光谱轮廓。在 230nm 激发下，详细讨论了来自 Pr 4f5d 态到其 4f 激发态的电子布居。随着 Pr 浓度的增加，PrP 和 D 发光具有不同的浓度相关特性。在共掺杂样品中掺入 Ce 会在 230nm 激发下产生强烈的 Ce 发光，这是 Pr 4f5d→Ce 5d ET 和 Ce 本征激发的综合结果。另一方面，Ce 5d→Pr 4f 的越来越强的 ET 导致 Ce 发射强度的降低，并且 Ce 发光衰减逐渐偏离系统中的单指数。通过采用 Inokuti-Hirayama 模型，确认偶极-偶极相互作用是控制此 ET 过程的主要多极效应，并且确定 C 值为 9.97×10^-29 m^2·s。最后，Ce 掺杂的 BaYSiO 材料的相对较低的闪烁光产率阻碍了其在闪烁体领域的应用潜力，而 Pr 的共取代导致闪烁性能的可观察下降。
