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Inorg Chem. 2018 Jun 18;57(12):7090-7096. doi: 10.1021/acs.inorgchem.8b00773. Epub 2018 Jun 4.

Site Occupation of Eu2+ in Ba2- xSr xSiO4 ( x = 0-1.9) and Origin of Improved Luminescence Thermal Stability in the Intermediate Composition.

Author information

1
MOE Key Laboratory of Bioinorganic and Synthetic Chemistry, KLGHEI of Environment and Energy Chemistry, School of Chemistry, School of Electronics and Information Technology , Sun Yat-sen University , Guangzhou 510275 , China.
2
Anhui Key Laboratory of Optoelectric Materials Science and Technology, Department of Physics , Anhui Normal University , Wuhu , Anhui 241000 , China.
3
The China-Germany Research Center for Photonic Materials and Device, State Key Laboratory of Luminescent Materials and Devices, and Guangdong Provincial Key Laboratory of Fiber Laser Materials and Applied Techniques, School of Materials Science and Engineering , South China University of Technology , Guangzhou 510641 , China.
4
Beijing Synchrotron Radiation Facility , Institute of High Energy Physics, Chinese Academy of Sciences , Beijing 100039 , China.

Abstract

Knowledge of site occupation of activators in phosphors is of essential importance for understanding and tailoring their luminescence properties by modifying the host composition. Relative site preference of Eu2+ for the two distinct types of alkaline earth (AE) sites in Ba1.9995- xSr xEu0.0005SiO4 ( x = 0-1.9) is investigated based on photoluminescence measurements at low temperature. We found that Eu2+ prefers to be at the 9-coordinated AE2 site at x = 0, 0.5, and 1.0, while at x = 1.5 and 1.9, it also occupies the 10-coordinated AE1 site with comparable preference, which is verified by density functional theory (DFT) calculations. Moreover, by combining low-temperature measurements of the heat capacity, the host band gap, and the Eu2+ 4f7 ground level position, the improved thermal stability of Eu2+ luminescence in the intermediate composition ( x = 1.0) is interpreted as due to an enlarged energy gap between the emitting 5d level and the bottom of the host conduction band (CB), which results in a decreased nonradiative probability of thermal ionization of the 5d electron into the host CB. Radioluminescence properties of the samples under X-ray excitation are finally evaluated, suggesting a great potential scintillator application of the compound in the intermediate composition.

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